In this work, we correlate network dynamics, supramolecular reversibility and the macroscopic surface scratch healing behavior for a series of elastomeric ionomers based on an amorphous backbone with varying fractions of carboxylate pendant groups completely neutralized by Na(+), Zn(2+) or Co(2+) as the counter ions. Our results based on temperature dependent dynamic rheology with simultaneous FTIR analysis clearly indicate that the effective supramolecular bond lifetime (τ(b)) is an important parameter to ascertain the ideal range of viscoelasticity for good macroscopic healing. The reversible coordination increased with higher valence metal ions and ionic content. Both rheological and spectroscopic analyses show a decrease in supramolecular assembly with temperature. The temperature dependent τ(b) was used to calculate the activation energy (Ea) of dissociation for the ionic clusters. According to self-healing experiments based on macroscale surface scratching, a supramolecular bond lifetime between 10 and 100 s results in samples with complete surface scratch healing and good mechanical robustness.

The utilization of dynamic covalent and noncovalent bonds in polymeric materials offers the possibility to regenerate mechanical damage, inflicted on the material, and is therefore of great interest in the field of self‐healing materials. For the design of a new class of self‐healing materials, methacrylate containing copolymers with acylhydrazones as reversible covalent crosslinkers are utilized. The self‐healing polymer networks are obtained by a bulk polymerization of an acylhydrazone crosslinker and commercially available methacrylates as comonomers to fine‐tune the Tg of the systems. The influence of the amount of acylhydrazone crosslinker and the self‐healing behavior of the polymers is studied in detail. Furthermore, the basic healing mechanism and the corresponding mechanical properties are analyzed.

Hydrogels have gained a lot of attention with their widespread use in different industrial applications. The versatility in the synthesis and the nature of the precursor reactants allow for a varying range of hydrogels with different mechanical and rheological properties. Understanding of the rheological behavior and the relationship between the chemical structure and the resulting properties is crucial, and is the focus of this review. Specifically, we include detailed discussion on the correlation between the rheological characteristics of hydrogels and their possible applications. Different rheological tests such as time, temperature and frequency sweep, among others, are described and the results of those tests are reported. The most prevalent applications of hydrogels are also discussed.

Traditional polyetherimides (PEIs) are commonly synthesized from an aromatic diamine and an aromatic dianhydride (e.g. 3,4'-oxydianiline (ODA) and 4,4'-oxydiphtalic anhydride (ODPA)) leading to the imide linkage and outstanding chemical, thermal and mechanical properties yet lacking any self-healing functionality. In this work, we have replaced the traditional aromatic diamine by a branched aliphatic fatty dimer diamine (DD1).This led to a whole family of self-healing polymers not containing reversible chemical bonds, capable of healing at (near) room temperature yet maintaining very high elastomeric-like mechanical properties (up to 6 MPa stress and 570% strain at break). In this work, we present the effect of the DD1/ODPA ratio on the general performance and healing behavior of a room temperature healing polyetherimide. A dedicated analysis suggests that healing proceeds in three steps: (i) an initial adhesive step leading to the formation of a relatively weak interface; (ii) a second step at long healing times leading to the formation of an interphase with different properties than the bulk material and (iii) disappearance of the damaged zone leading to full healing. We argue that the fast interfacial adhesive step is due to van der Waals interactions of long dangling alkyl chains followed by an interphase formation due to polymer chain interdiffusion. An increase in DD1 ratio leads to an increase in the healing kinetics and displacement shift of the first healing step towards lower temperatures. An excess of DD1 leads to the crosslinking of the polymer thereby restricting the necessary mobility for the interphase formation and limiting the self-healing behavior. The results here presented offer a new route for the development of room temperature self-healing thermoplastic elastomers with improved mechanical properties using fatty dimer diamines.

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In this work, pendant groups with both furan and maleimide moieties were incorporated into a polymethacrylate copolymer with lauryl methacrylate as comonomer to yield a one‐system Diels–Alder (DA) polymer. A combined Fourier transform infrared (FTIR) spectroscopy and rheological study was performed to quantify the extent of the reversible DA reaction and the resulting changes in mechanical properties of the polymer. The kinetics of the retro‐Diels–Alder (rDA) reaction was studied at different temperatures to determine an enthalpy of activation. Control polymers with only one functional moiety, that is, the furan or maleimide, were also synthesized to study the differences in viscoelastic behavior and the absence of self‐healing. Microscratch tests were performed to obtain information about the disappearance of well‐defined intentional surface scratches under different healing conditions. © 2014 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2014, 52, 1669–1675

The healing phenomenon of metallopolymers is studied in detail and the dependency of the chosen metal salt is provided. Furthermore, a correlation between the supramolecular bond life time and the healing behavior could be revealed.

This article reviews some of the intrinsic self-healing epoxy materials that have been investigated throughout the course of the last twenty years. Emphasis is placed on those formulations suitable for the design of high-performance composites to be employed in the aerospace field. A brief introduction is given on the advantages of intrinsic self-healing polymers over extrinsic counterparts and of epoxies over other thermosetting systems. After a general description of the testing procedures adopted for the evaluation of the healing efficiency and the required features for a smooth implementation of such materials in the industry, different self-healing mechanisms, arising from either physical or chemical interactions, are detailed. The presented formulations are critically reviewed, comparing major strengths and weaknesses of their healing mechanisms, underlining the inherent structural polymer properties that may affect the healing phenomena. As many self-healing chemistries already provide the fundamental aspects for recyclability and reprocessability of thermosets, which have been historically thought as a critical issue, perspective trends of a circular economy for self-healing polymers are discussed along with their possible advances and challenges. This may open up the opportunity for a totally reconfigured landscape in composite manufacturing, with the net benefits of overall cost reduction and less waste. Some general drawbacks are also laid out along with some potential countermeasures to overcome or limit their impact. Finally, present and future applications in the aviation and space fields are portrayed.