Self-healing polymeric materials are systems that after damage can revert to their original state with full or partial recovery of mechanical strength. Using scaling theory we study a simple model of autonomic self-healing of unentangled polymer networks. In this model one of the two end monomers of each polymer chain is fixed in space mimicking dangling chains attachment to a polymer network, while the sticky monomer at the other end of each chain can form pairwise reversible bond with the sticky end of another chain. We study the reaction kinetics of reversible bonds in this simple model and analyze the different stages in the self-repair process. The formation of bridges and the recovery of the material strength across the fractured interface during the healing period occur appreciably faster after shorter waiting time, during which the fractured surfaces are kept apart. We observe the slowest formation of bridges for self-adhesion after bringing into contact two bare surfaces with equilibrium (very lo...

/pdf/self-healing-of-unentangled-polymer-networks-with-reversible-1h05vmohxn.pdf

Self-Healing of Unentangled Polymer Networks with Reversible Bonds.

A review on self-healing polymers for soft robotics

An innovative type of connections for glass components, called laminated connections, has been developed in the last years. Two materials have been used for laminated connections: the transparent ionomer SentryGlas® (SG) from Kuraray (former Dupont) and the Transparent Structural Silicon Adhesive (TSSA) from Dow Corning. In this paper, the mechanical behaviour of SG and TSSA bulk materials is studied under uniaxial tensile stress condition. The effects of strain rate and temperature variations are investigated. Particular attention is paid (i) to the study of these polymers in cured condition and (ii) to the computation of true stress and strain field during the tests. Firstly, it is observed that the mechanical behaviour of both SG and TSSA are temperature and strain rate dependent. These effects are quantitatively determined in the paper. Secondly, two additional phenomena are observed. For TSSA, it is observed that the material goes from fully transparent to white colour, exhibiting the so-called whitening phenomenon. For SG, instead, it is observed that the strain field distribution is dependent on the temperature. More specifically, the material exhibits a non-uniform strain field distribution due to the occurring of the necking phenomenon. Measurements along the specimens, using Digital Image Correlation techniques, showed that the localized strain propagates over the full specimen length, resulting in a cold-drawing phenomenon. Finally, it is also shown that engineering and true stress–strain definition exhibits large deviation indicating that the finite deformation theory should be used for the computation of the stress–strain curves to be implemented in numerical modelling.

/pdf/the-mechanical-behaviour-of-sentryglas-ionomer-and-tssa-3ui07sdij5.pdf

The mechanical behaviour of SentryGlas® ionomer and TSSA silicon bulk materials at different temperatures and strain rates under uniaxial tensile stress state

Particulate materials loaded under uniaxial compression and tension are studied using the discrete element method. Self-healing of the damaged samples is activated through sintering, a process that effectively increases the contact adhesion (i.e. the tensile strength) between particles. The initial sample is prepared from spherical particles by applying high (isotropic) pressure, where particles in contact deform plastically and adhere to each other due to increased van der Waals forces. The result of this pressure-sintering is a solid sample from which the stress is released before uniaxial tension or compression is applied. Damage occurs “microscopically” through loss of contacts and thus loss of adhesion. In order to “self-heal” (part of) this damage, the system is sintered again, so that the adhesion at existing contacts in the damaged sample becomes stronger than originally. The stress–strain curves for the mechanically loaded samples are characterised by a peak-strength followed by a softening branch. Self-healing of an originally “weak” sample, up to a “strong” adhesion level, leads to qualitatively different stress–strain behaviour, dependent on the strain at which self-healing is applied. Interestingly, the response of the “weak” self-healed material is bounded by the damage response of the “strong” material. For an optimal self-healing of the particulate material, it is preferable to initiate the healing mechanism during the early stage of damage development, before the peak-strength is reached.

/pdf/self-healing-of-damaged-particulate-materials-through-5obsrrryf0.pdf

Self-healing of damaged particulate materials through sintering

Permanent polymer networks present an important sustainability challenge. Irreversible covalent crosslinks impart these materials excellent mechanical properties, thermal and chemical resistance, yet also render them difficult to repair and to recycle. Self-healing mechanisms can extend the lifetime of thermosets and elastomers, improving their durability and making their lifecycle more sustainable. In addition to the lifetime extension, this paper reviews the sustainability of self-healing polymers from a holistic point of view. The entire lifecycle of self-healing polymers is critically assessed with reference to the green chemistry principles and sustainable development. The relation between the self-healing chemistries and the sustainability aspects of each of the phases of the lifecycle are discussed, starting from the feedstocks, monomer functionalisation and polymer synthesis, to processing and manufacturing as well as end-of-life considerations, i.e. recycling or (bio)degradation. The review provides a toolbox for the development of more sustainable thermosets, elastomers and their composites. It is of utmost importance to consider the entire lifecycle of self-healing materials, derived products and – by extension – any material or product. The self-healing ability and often related recyclability should primarily reduce the amount of new materials that are necessary to fulfill societal needs, by extending the lifetime of products and maximizing reprocessing into new products. Increasing healing efficiency and the number of healing cycles improves the overall environmental impact relative to the extended service lifetime. Renewable resources derived from biomass, recycling processes or waste streams should be the first choice to create new self-healing polymers. Finally, biodegradability can be considered as a complementary end-of-life scenario upon accidental loss of self-healing polymer to the environment, provided that the biodegradation does not start under the prospected use conditions of the self-healing polymers and products, but can be postponed until contact with stimuli present in the environment. 

Sustainability of self-healing polymers: A holistic perspective towards circularity in polymer networks

lonomers are a class of polymers that have up to 20mol% of ionic species incorporated into the structure of organic polymer. These ionic species create interactions that are not possible in non-ionic polymers. These have profound effect on mechanical and physical properties of the polymer. Bonded to the backbone, these polymers show self-healing property when incurred to damage.

Ionomers: The Self-healing Polymers

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Ionomers: The Self-healing Polymers