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Self-Healing Materials and Devices
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Self-Healing Materials and Devices

A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Materials Chemistry".

Deadline for manuscript submissions: closed (10 July 2022) | Viewed by 14744

Special Issue Editors

Prof. Dr. Xinxing Zhang

E-Mail Website
Guest Editor
State Key Laboratory of Polymer Materials Engineering, Polymer Research Institute of Sichuan University, Chengdu 610065, China
Interests: self-healing; supramolecular chemistry; polymer nanocomposites; sensors; actuators
Dr. Doina Dimonie

E-Mail Website
Guest Editor
National Institute for Research and Development in Chemistry and Petrochemistry, 060021 Bucharest, Romania
Interests: polymers; polymer modifications; polymeric compounds; polymeric composites; polymeric nanocomposites; 3D printing; designed functional properties for target applications

Special Issue Information

Dear Colleagues,

Polymers are undoubtedly excellent candidates for the design of self-healing materials, which have the ability to repair or restore damage, due to their widespread application and various self-healing mechanisms. Specifically, the underlying healing mechanisms can be categorized into extrinsic and intrinsic self-healing materials. Extrinsic self-healing materials rely on the healing agents (via catalysis or reactive precursors) encapsulated in the capsule or vascular network of the polymer substrate, which would automatically be released in damaged regions and then trigger the polymeric polymerization or crosslinking reaction to enable the self-repair of the fractures. On the other hand, intrinsic self-healing materials are enabled by introducing reversible noncovalent or dynamic covalent interactions in the polymer matrix, such as hydrogen bonding, metal–ligand coordination interactions, ionic interactions, π–π interactions, disulfide bonds, and dynamic boroxine bonding. Moreover, endowing devices with a self-healing ability is of significance to achieving a long lifetime and reducing polymer waste, especially in the circular economy model. Over the past few decades, tremendous progress has been made in the development of self-healing materials, which have been successfully integrated into different functional devices, including sensors, artificial muscle, solar cells, field-effect transistors, dielectric actuators, and energy devices. The aim of this Special Issue is to provide readers with an up-to-date overview of recent progress in research on self-healing materials and devices.

Prof. Dr. Xinxing Zhang
Dr. Doina Dimonie
Guest Editors

Manuscript Submission Information

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Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 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

  • self-healing
  • functional devices
  • supramolecular chemistry
  • reversible crosslink
  • dynamic bond
  • reversible bond

Published Papers (6 papers)

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Research

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10 pages, 2558 KiB  
Article
Mechanically Robust Dual-Crosslinking Elastomer Enabled by a Facile Self-Crosslinking Approach
by Zhendong Huang, Biqiang Jin, Haitao Wu, Zihang Zeng, Minghui Huang, Jinrong Wu, Lusheng Liao and Jing Zheng
Materials 2022, 15(11), 3983; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15113983 - 03 Jun 2022
Viewed by 1769
Abstract
We propose a simple but rapid strategy to fabricate self-crosslinked dual-crosslinking elastomers (SCDCEs) with high mechanical properties. The SCDCEs are synthesized through one-pot copolymerization of Butyl acrylate (BA), acrylic amide (AM), and 3-Methacryloxypropyltrimethoxysilane (MEMO). Both the amino group on AM and the methoxy [...] Read more.
We propose a simple but rapid strategy to fabricate self-crosslinked dual-crosslinking elastomers (SCDCEs) with high mechanical properties. The SCDCEs are synthesized through one-pot copolymerization of Butyl acrylate (BA), acrylic amide (AM), and 3-Methacryloxypropyltrimethoxysilane (MEMO). Both the amino group on AM and the methoxy group on MEMO can be self-crosslinked after polymerization to form a dual-network crosslink consisting of hydrogen bonds crosslink and Si-O-Si covalent bonds crosslink. The SCDC endow optimal elastomer with high mechanical properties (the tensile strength is 6MPa and elongation at break is 490%) as the hydrogen bonds crosslink can serve as sacrificial construction to dissipate stress energy, while covalent crosslinking networks can ensure the elasticity and strength of the material. These two networks also contribute to the recoverability of the elastomers, leading them to recover their original shape and mechanical properties after being subjected to deformation in a short time. Full article
(This article belongs to the Special Issue Self-Healing Materials and Devices)
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13 pages, 4397 KiB  
Article
Ultra-Stretchable and Self-Healing Anti-Freezing Strain Sensors Based on Hydrophobic Associated Polyacrylic Acid Hydrogels
by Shuya Yin, Gehong Su, Jiajun Chen, Xiaoyan Peng and Tao Zhou
Materials 2021, 14(20), 6165; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14206165 - 18 Oct 2021
Cited by 4 | Viewed by 1902
Abstract
Water-rich conductive hydrogels with excellent stretchability are promising in strain sensors due to their potential application in flexible electronics. However, the features of being water-rich also limit their working environment. Hydrogels must be frozen at subzero temperatures and dried out under ambient conditions, [...] Read more.
Water-rich conductive hydrogels with excellent stretchability are promising in strain sensors due to their potential application in flexible electronics. However, the features of being water-rich also limit their working environment. Hydrogels must be frozen at subzero temperatures and dried out under ambient conditions, leading to a loss of mechanical and electric properties. Herein, we prepare HAGx hydrogels (a polyacrylic acid (HAPAA) hydrogel in a binary water–glycerol solution, where x is the mass ratio of water to glycerol), in which the water is replaced with water–glycerol mixed solutions. The as-prepared HAGx hydrogels show great anti-freezing properties at a range of −70 to 25 °C, as well as excellent moisture stability (the weight retention rate was as high as 93% after 14 days). With the increase of glycerol, HAGx hydrogels demonstrate a superior stretchable and self-healing ability, which could even be stretched to more than 6000% without breaking, and had a 100% self-healing efficiency. The HAGx hydrogels had good self-healing ability at subzero temperatures. In addition, HAGx hydrogels also had eye-catching adhesive properties and transparency, which is helpful when used as strain sensors. Full article
(This article belongs to the Special Issue Self-Healing Materials and Devices)
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14 pages, 3350 KiB  
Article
Dual Covalent Cross-Linking Networks in Polynorbornene: Comparison of Shape Memory Performance
by Haotian Zhao, Qinghong Zhang, Xinlong Wen, Gongliang Wang, Xiaowen Gong and Xinyan Shi
Materials 2021, 14(12), 3249; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14123249 - 12 Jun 2021
Cited by 3 | Viewed by 1830
Abstract
In this work, tetrakis(dimethyllamino)ethylene (TDAE) plasticized polynorbornene (PNB) was used as the matrix, sulfur (S) and dicumyl peroxide (DCP) were simultaneously used as crosslinking agents to construct dual covalent cross-linking networks in PNB. The effects of different amounts of cross-linkers on the crosslinking [...] Read more.
In this work, tetrakis(dimethyllamino)ethylene (TDAE) plasticized polynorbornene (PNB) was used as the matrix, sulfur (S) and dicumyl peroxide (DCP) were simultaneously used as crosslinking agents to construct dual covalent cross-linking networks in PNB. The effects of different amounts of cross-linkers on the crosslinking degree, mechanical property, glass transition temperature, and PNB shape memory performance were investigated. Two crosslinking mechanisms were examined by Fourier transform infrared spectrometer and Raman spectrometer. The results showed that sulfur-rich cross-linked PNB exhibited a higher crosslinking degree, tensile strength, and slightly higher glass transition temperature than the DCP-rich system. Cross-linked PNB presented better shape memory performance than the uncross-linked one. Sulfur-rich cross-linked PNB showed even better shape memory behavior than the DCP-rich system, both with a shape fixation ratio of over 99% and a shape recovery ratio of over 90%. The reaction mechanism of sulfur and DCP in cross-linking PNB was different. Sulfur reacted with the α-H in PNB to form monosulfide bonds, disulfide bonds, and polysulfide bonds in PNB and the number of polysulfide bonds increased with increased amounts of sulfur. DCP reacted with the double bonds in PNB to form C-C covalent bond crosslinking networks. The crosslinking mechanism revealed that the sulfur-containing cross-linked bonds, especially polysulfide bonds, were more flexible and bore large deformation, which gave the PNB excellent mechanical properties and ensured a higher shape entropy elastic recovery ratio. Full article
(This article belongs to the Special Issue Self-Healing Materials and Devices)
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13 pages, 3492 KiB  
Article
Fabrication and Property Regulation of Small-Size Polyamine Microcapsules via Integrating Microfluidic T-Junction and Interfacial Polymerization
by Shaochuan Lai, Yongjun He, Daoying Xiong, Yao Wang, Kaibin Xiao, Zhibin Yan and He Zhang
Materials 2021, 14(7), 1800; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14071800 - 05 Apr 2021
Cited by 4 | Viewed by 2157
Abstract
The self-healing system based on microencapsulated epoxy-amine chemistry is currently the self-healing system with the most practical application potential. It can be widely used in many epoxy-based materials with a size restriction for the microcapsules, such as fiber-reinforced composites, anti-corrosion coatings, etc. Although [...] Read more.
The self-healing system based on microencapsulated epoxy-amine chemistry is currently the self-healing system with the most practical application potential. It can be widely used in many epoxy-based materials with a size restriction for the microcapsules, such as fiber-reinforced composites, anti-corrosion coatings, etc. Although epoxy microcapsules of different sizes can be fabricated using different techniques, the preparation of polyamine microcapsules with suitable sizes and good performance is the prerequisite for further developing this self-healing system. In this investigation, based on the novel microencapsulation technique via integrating microfluidic T-junction and interfacial polymerization, the feasibility of preparing small-size polyamine microcapsules and the process regulation to optimize the properties of the small-size microcapsules were studied. We show that polyamine microcapsules with sizes smaller than 100 μm can be obtained through the T-junction selection and the feeding rate control of the polyamine. To regulate the small-size microcapsules’ quality, the effects of the concentration of the shell-forming monomer and the solvent with different polarity in the reaction solution and the reaction condition were studied. It shows that dry, free-flowing small-size microcapsules can still be obtained when the shell-forming monomer concentration is higher and the solvent’s polarity is lower, compared with the preparation of larger polyamine microcapsules. Although the change of reaction conditions (reaction temperature and duration) has a certain effect on the microcapsules’ effective core content, it is relatively small. The results of this investigation further promote the potential application of the self-healing systems based on microencapsulated epoxy-amine chemistry in materials with a size restriction for the microcapsules. Full article
(This article belongs to the Special Issue Self-Healing Materials and Devices)
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11 pages, 2254 KiB  
Article
Dynamic Crosslinking: An Efficient Approach to Fabricate Epoxy Vitrimer
by Yin Ran, Ling-Ji Zheng and Jian-Bing Zeng
Materials 2021, 14(4), 919; https://0-doi-org.brum.beds.ac.uk/10.3390/ma14040919 - 15 Feb 2021
Cited by 12 | Viewed by 3228
Abstract
Epoxy vitrimers with reprocessability, recyclability, and a self-healing performance have attracted increasingly attention, but are usually fabricated through static curing procedures with a low production efficiency. Herein, we report a new approach to fabricate an epoxy vitrimer by dynamic crosslinking in a torque [...] Read more.
Epoxy vitrimers with reprocessability, recyclability, and a self-healing performance have attracted increasingly attention, but are usually fabricated through static curing procedures with a low production efficiency. Herein, we report a new approach to fabricate an epoxy vitrimer by dynamic crosslinking in a torque rheometer, using diglycidyl ether of bisphenol A and sebacic acid as the epoxy resin and curing agent, respectively, in the presence of zinc acetylacetonate as the transesterification catalyst. The optimal condition for fabricating the epoxy vitrimer (EVD) was dynamic crosslinking at 180 °C for ~11 min. A control epoxy vitrimer (EVS) was prepared by static curing at 180 °C for ~11 min. The structure, properties, and stress relaxation of the EVD and EVS were comparatively investigated in detail. The EVS did not cure completely during static curing, as evidenced by the continuously increasing gel fraction when subjected to compression molding. The gel fraction of the EVD did not change with compression molding at the same condition. The physical, mechanical, and stress relaxation properties of the EVD prepared by dynamic crosslinking were comparable to those of the EVS fabricated by static curing, despite small differences in the specific property parameters. This study demonstrated that dynamic crosslinking provides a new technique to efficiently fabricate an epoxy vitrimer. Full article
(This article belongs to the Special Issue Self-Healing Materials and Devices)
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Review

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30 pages, 10444 KiB  
Review
Recent Advances in Electronic Skins with Multiple-Stimuli-Responsive and Self-Healing Abilities
by Quanquan Guo, Xiaoyan Qiu and Xinxing Zhang
Materials 2022, 15(5), 1661; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15051661 - 23 Feb 2022
Cited by 8 | Viewed by 2760
Abstract
Wearable electronic skin (e-skin) has provided a revolutionized way to intelligently sense environmental stimuli, which shows prospective applications in health monitoring, artificial intelligence and prosthetics fields. Drawn inspiration from biological skins, developing e-skin with multiple stimuli perception and self-healing abilities not only enrich [...] Read more.
Wearable electronic skin (e-skin) has provided a revolutionized way to intelligently sense environmental stimuli, which shows prospective applications in health monitoring, artificial intelligence and prosthetics fields. Drawn inspiration from biological skins, developing e-skin with multiple stimuli perception and self-healing abilities not only enrich their bionic multifunctionality, but also greatly improve their sensory performance and functional stability. In this review, we highlight recent important developments in the material structure design strategy to imitate the fascinating functionalities of biological skins, including molecular synthesis, physical structure design, and special biomimicry engineering. Moreover, their specific structure-property relationships, multifunctional application, and existing challenges are also critically analyzed with representative examples. Furthermore, a summary and perspective on future directions and challenges of biomimetic electronic skins regarding function construction will be briefly discussed. We believe that this review will provide valuable guidance for readers to fabricate superior e-skin materials or devices with skin-like multifunctionalities and disparate characteristics. Full article
(This article belongs to the Special Issue Self-Healing Materials and Devices)
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