The evolution of self-healing polymers has resulted in a myriad of healing designs that have given way to complex systems capable of supporting multiple cycles, among other features. This progression enables us to propose the implementation of a timeline that classifies self-healing polymers in generations based on the healing mechanism, and correlated with historical development. The first generation employed the encapsulation of external healing agents; the second one, based on intrinsic mechanisms, applied reversible chemistries; and the third generation was inspired by natural examples such as plants and human skin, in which the healing agent is embedded in vascular networks. Despite great efforts and, with a few exceptions, polymers with high healing efficiency and high mechanical performance are not common. To improve this situation, a combination of different mechanisms is currently emerging, giving birth to the fourth generation of self-healing materials. This article, focused on self-healing elastomers, provides a rigorous overview of this new generation, in which the combination of covalent bonds and non-covalent interactions provides an optimal balance between mechanical performance and repairability. The implementation of this concept leads to materials with real commercial potential in functional applications, such as coatings, sensors, actuators, controlled release of drugs, seals, gaskets, hoses, and even high-performance applications such as tires and railway components.

/pdf/evolution-of-self-healing-elastomers-from-extrinsic-to-2ng2zi4az8.pdf

Evolution of self-healing elastomers, from extrinsic to combined intrinsic mechanisms: a review

A review on self-healing polymers for soft robotics

Replicating nacre’s multiscale architecture represents a promising approach to design artificial materials with outstanding rigidity and toughness. It is highly desirable yet challenging to incorporate self-healing and shape-programming capabilities into nacre-mimetic composites due to their rigidity and high filler content. Here, we report such a composite obtained by infiltrating a thermally switchable Diels-Alder network polymer into a lamellar scaffold of alumina. The chemical bond switchability and the physical confinement by the filler endows the composite with sufficient molecular mobility without compromising its thermal dimension stability. Consequently, our composite is capable of self-healing internal damages. Additionally, in contrast to the intractable planar shape of other artificial nacres, precise control of the polymer chain dynamics allows the shape of our composite to be programmed permanently via plasticity and temporarily via shape memory effect. Our approach paves a new way for designing durable multifunctional bioinspired structural materials. Incorporation of self-healing and shape programming capabilities into rigid, structural composite is highly desirable yet challenging. Here, the authors report a nacre-mimetic composite obtained by infiltrating a switchable Diels-Alder network polymer into a scaffold of alumina capable of self-healing internal damage.

/pdf/nacre-mimetic-composite-with-intrinsic-self-healing-and-2l6w9g9dnx.pdf

Nacre-mimetic composite with intrinsic self-healing and shape-programming capability.

A high stiffness and self-healable polyurethane based on disulfide bonds and hydrogen bonding

Significant advances have been made in the development of self-healing synthetic polymer materials in recent years. This review article discusses the recent progress in preparation, characterization and properties of different kinds of intrinsic self-healing elastomers based on reversible covalent bonds and dynamic supramolecular chemistry. Healing conditions, mechanical property recovery and healing efficiency are the main discussion topics. Potential applications, challenges and future prospects in self-healing elastomer fields are also discussed in the last part of this review.

Preparation, characterization and properties of intrinsic self-healing elastomers

Self-healing behavior of polyurethanes based on dual actions of thermo-reversible Diels-Alder reaction and thermal movement of molecular chains

Given its thermal reversibility, high yield, and minimal side reactions, the Diels–Alder (DA) reaction is a particularly desirable technique for the preparation of polymeric materials with heat-stimulated self-healing properties. A linear self-healing polyurethane containing thermally reversible DA bonds (PU-DA) was developed in this study. Results revealed that the introduction of DA bonds conferred outstanding mechanical property and thermal reversibility to PU-DA films. Thus, the as-prepared PU-DA films demonstrated excellent self-healing performance. The self-healing behavior of the PU-DA films under various heat treatments was examined through qualitative observation and quantitative measurements. The PU-DA underwent self-repair through the combination of two healing actions, i.e., the thermal movement of molecular chains and the thermally reversible DA reaction. Moreover, the self-healing behavior of the PU-DA was repeatable, and the PU-DA continued to present high strength even after undergoing three damage–repair cycles at the same site. In addition, the as-prepared PU-DA exhibited excellent macro-scale self-healing behavior, and it endowed the PU-DA presented reprocessing performance. The PU-DA can be recycled given its excellent self-healing and outstanding reprocessing performances.

Effect of Heat-Treatment on Self-healing and Processing Behavior of Thermally Reversible Polyurethanes

Effect of failure modes on healing behavior and multiple healing capability of self-healing polyurethanes

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Self-healing behavior of polyurethanes based on dual actions of thermo-reversible Diels-Alder reaction and thermal movement of molecular chains

Effect of Heat-Treatment on Self-healing and Processing Behavior of Thermally Reversible Polyurethanes

Effect of failure modes on healing behavior and multiple healing capability of self-healing polyurethanes