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Tactile texture sensors are designed to evaluate the sensations felt when a human touches an object. Prior studies have demonstrated the necessity for these sensors to have compliant ridges on their surfaces that mimic human fingerprints. These features enable the simulation of contact phenomena, especially friction and vibration, between human fingertips and objects, enhancing the tactile sensation evaluation. However, the ridges on tactile sensors are susceptible to abrasion damage from repeated use. To date, the healing function of abraded ridges has not been proposed, and its effectiveness needs to be demonstrated. In this study, we investigated whether the signal detection capabilities of a sensor with abraded epidermal ridges could be restored by healing the ridges using polyvinyl chloride plastisol as the sensor material. We developed a prototype tactile sensor with an embedded strain gauge, which was used to repeatedly scan roughness specimens. After more than 1000 measurements, we observed significant deterioration in the sensor's output signal level. The ridges were then reshaped using a mold with a heating function, allowing the sensor to partially regain its original signal levels. This method shows potential for extending the operational lifespan of tactile texture sensors with compliant ridges. [ABSTRACT FROM AUTHOR]

In this study, we investigate a self-healing 60Pb40Sn reinforced Al6061 alloy's tribological behavior through experimentation, focusing on the influence of different reinforcement concentrations on tribological performance. Cylindrical pins with varying filler concentrations were tested using a pin-on-roller Tribometer to evaluate friction behavior, wear resistance, and fractured surface morphology. The results revealed intriguing findings, including a 5% higher coefficient of friction (COF) for the maximum solder concentration sample at lower loads and speeds. Under higher loads (100 N), the COF increased by approximately 16%. However, the three-hole pin samples consistently exhibited higher weight loss than the two-hole pins. Remarkably, at a 100 N load and extended sliding distances, the three-hole pins showed slightly lower friction values, with a reduced COF of 12%, 16%, and 12% at 53 rpm, 106 rpm, and 160 rpm, respectively. Morphological characterization using Scanning Electron Microscope (SEM), Energy Dispersive Spectrum (EDS), and Elemental Maps revealed the wear mechanism and oxidation on the pins' surfaces, contributing to enhanced wear resistance in this self-healing composite, thus presenting a novel insight into self-healing alloy tribology. [ABSTRACT FROM AUTHOR]

The paper presents an enhanced version of an arc electron source designed for air ionization applications in a self-neutralizing air-breathing plasma thruster. The arc electron source is specifically suited for the air-breathing plasma thruster, as it allows precise control of mean electron energy levels. This paper focuses on the ionization aspects of air-breathing thrusters through the development of axially magnetized arc electron sources. The sources consist of a circular and coaxial configuration of a metallic arc plasma source coupled with a positively biased grid to extract electrons and control mean electron energy. The average mean electron energy of electrons in the arc electron source is regulated by adjusting the bias voltage of the grid within the range of 0 V – 300 V. To investigate the behavior of ion current density and electron density concerning pressure and mean electron energy, the current probe and magnetic filter were utilized. It was demonstrated that the circular electron source leads to enhanced ionization of airflow by achieving plasma densities greater than 1018 m−3. By utilizing a high-speed camera for the circular arc electron source, the arc spot was seen to move azimuthally due to the magnetic field. Furthermore, scanning electron microscopy and a conductance measurement system were employed for the coaxial arc electron source to examine the deposition and conductance of the electron extraction grid. While the grid underwent deposition of about 600 microns, the conductance was observed to increase/saturate with time and bias voltage, indicating an electrically "self-healing material". [ABSTRACT FROM AUTHOR]

Maintaining the health and reliability of civil facilities is of strategic importance. In highway engineering, pavement cracking impairs the road service and travel comfort level, while structure cracking can cause catastrophic damage. Microcapsule-based self-healing materials offer solutions to auto-recovery micro-cracks and maintain structural health. Such solution has become available by laboratory synthesis and proved effective in addressing the cracking problem during long-term mechanical, thermal, and hydraulic conditions. However, full-scale applications of this technique are not prevalent, showing its potential limitations in highway engineering. Crack healing in highways is a big topic, therefore, this review has two insertion points. (1) We focus on the cracking issues on two specific materials: asphalt and concrete, which account for the vast majority of all the materials used in pavement and structures in highways. (2) Instead of the laboratory studies, we pay more attention to the practical applications, the meaning of healing performance, and the adverse effects of microcapsules to the main structural components (i.e., tunnel lining, bridge piers and beams) and pavement in highways. The practical significance of self-healing materials in highway projects was discussed from the three aspects: strength, durability, and stress redistribution. The difficulty in applying this new technique is also discussed from economic perspective. For future-proofing, a material evaluation system that fits the load condition is required. The self-healing technique brings composites a chance to interact with the environment, showing high potential for contributing to the development of various types of long-lasting infrastructures.

Tactile texture sensors are designed to evaluate the sensations felt when a human touches an object. Prior studies have demonstrated the necessity for these sensors to have compliant ridges on their surfaces that mimic human fingerprints. These features enable the simulation of contact phenomena, especially friction and vibration, between human fingertips and objects, enhancing the tactile sensation evaluation. However, the ridges on tactile sensors are susceptible to abrasion damage from repeated use. To date, the healing function of abraded ridges has not been proposed, and its effectiveness needs to be demonstrated. In this study, we investigated whether the signal detection capabilities of a sensor with abraded epidermal ridges could be restored by healing the ridges using polyvinyl chloride plastisol as the sensor material. We developed a prototype tactile sensor with an embedded strain gauge, which was used to repeatedly scan roughness specimens. After more than 1000 measurements, we observed significant deterioration in the sensor’s output signal level. The ridges were then reshaped using a mold with a heating function, allowing the sensor to partially regain its original signal levels. This method shows potential for extending the operational lifespan of tactile texture sensors with compliant ridges.

In this study, we report the enhanced electrochemical performance of a MnO2 electrode modified with a pH-sensitive co-polymer, activated at acidic pH, and designed to counteract MnO2 degradation in aqueous aqueous pseudocapacitors. The conformation of this polymer is controlled by the local pH changes that occur at the electrode/electrolyte interface during electrochemical stress associated to oxygen evolution.As a proof of concept, we demonstrate that the addition of the pH-sensitive polymer contributes to improved electrode integrity and lifetime under over-polarization with oxygen evolution. After undergoing 10 cycles of electrochemical stress, the MnO2/pH-sensitive polymer composite retains ∼ 70 % of its capacitance. This remarkable result stands in stark contrast with the pristine MnO2 electrode which fails catastrophically under the same stress conditions. We believe that this pH-induced self-protection mechanism represents a significant advancement in the development of novel smarter self-healing electroactive materials for the next generation of energy storage devices.

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There is a category of materials known as self-healing materials, which are distinguished by their inherent capacity to mend themselves in the event of internal damage or fractures. Because it possesses a built-in healing mechanism, it possesses this one-of-a-kind power. This system can react to injury in methods that range encompassing chemical reactions, physical alterations, and biological processes. The need to extend the endurance and longevity of materials used in a variety of industries, such as building, transportation, and electronics, has been a driving force behind the creation of self-healing materials. The mechanisms that are used to research self-healing materials as well as the approaches that are used to characterise them are discussed in this article. The many methods of self-healing, such as microcapsule-based healing, intrinsic healing, and extrinsic healing, are explored in this article. Intrinsic healing is also covered. In addition, the characterization methods that were utilised in order to evaluate the efficacy of the healing process, such as mechanical assessment, thermal evaluation, and microscopy, are discussed here. In addition, the prospective usages for self-healing materials in several industries, such as coatings, adhesives and related products composites, and biomedical devices, are addressed in this article. In this article, the advantages of using self-healing materials in certain applications are described such as an improvement in the materials' longevity, reliability, and sustainability.

Summary: Two significant drawbacks of current self‐healing materials are that they are: (1) Passive and as such do not guarantee a match between the healing and damage rate; (2) Not monitored during and after healing, so that the performance of the healed material is not known without retrospective offline testing. As a consequence their application is currently limited in some sectors, such as the aerospace sector where high performance needs to be guaranteed within strict guidelines. This article proposes the first active self‐healing material that integrates with control and fault diagnosis to provide a system with a desired healing response. A fault diagnosis algorithm using supervised regression is used to estimate the measure of damage. Then based on this estimate, adaptive feedback control is used to ensure a match between the healing response and the damage rate, while taking into account the nonlinear system dynamics and uncertainty. The system is demonstrated in simulation using a self‐healing material based on piezoelectricity and electrolysis. This shows the ability of the integrated subsystems to tackle these two significant drawbacks of most current self‐healing systems and will benefit applications with strict performance requirements, or systems operating under harsh conditions or that are remotely accessed. [ABSTRACT FROM AUTHOR]

This study presents a comparative analysis of different sustainable alternatives for producing reinforced ionic elastomers that are not just mechanically robust but also excellent in recyclability and self-healing, marking a significant advancement in sustainable materials science. Ionically crosslinked carboxylated nitrile rubber (XNBR) was combined with conventional (carbon black and silica) and sustainable (cellulose and ground tire rubber) fillers. The sustainable fillers not only enhanced the mechanical performance (reinforcing character) but also maintained high healing efficiencies (>80 %). Notably, the incorporation of just 10 phr of waste-based ground tire rubber (GTR) produced by water jet grinding (WJ-GTR) resulted in a material capable of complete repair and recycling (100 % efficiency) after temperature-driven protocols, with mechanical properties and a reinforcement index comparable to those of conventional fillers such as silica. This achievement represents a major breakthrough in the field of sustainable composites, as it offers a unique blend of robust mechanical properties and environmental sustainability. [Display omitted] • Reinforced, recyclable and self-healable ionic elastomers (XNBR) are developed. • Cellulose and ground tire rubber (GTR) are explored as sustainable fillers. • Incorporation of 10 phr GTR results in a fully recyclable and repairable rubber. • Reinforcement index is comparable to that of conventional fillers like silica. [ABSTRACT FROM AUTHOR]

Extrinsic self-healing corrosion protective coatings have attracted substantial interest because of their ability to prevent damage propagation by releasing corrosion inhibitors and polymerizable agents from micro/nanocarriers. Various micro/nanoencapsulation technologies have been adopted to optimize the loading capacity and to control the releasing behavior of the healing agents for enhancing the self-healing functionality. This study aims to review recent advances in self-healing corrosion protective coatings based on micro/nanocarriers. This review also provides insights for the further development of extrinsic self-healing coatings by evaluating the advantages and limitations of different healing systems.

Conformal integration of electronics on complex curvilinear surfaces remains challenging, especially for those devices made of non‐stretchable materials. Transforming as‐fabricated planar sheets onto curved surfaces requires the materials to be flexible and stretchable, which is intrinsically in conflict with the nature of non‐stretchable materials. Here, a novel assembly strategy for conformal electronics is proposed that utilizes kirigami design at the structural level for the non‐stretchable planar sheets to conformally and completely wrap the curved surfaces, and employs self‐healing materials to connect the sheets at the seams. Conductive self‐healing materials are used to ensure the electrical conductivity of the functional materials so as to assure device functionality. The transformation from a planar kirigami sheet to a sphere surface demonstrates this strategy, which is designed and predicted by theoretical and numerical studies and realized by experiments. Simple examples such as a conformal heater and a multifunctional wind sensing system on a spherical surface demonstrate the wide potential applications of the proposed strategy. [ABSTRACT FROM AUTHOR]

An integration of flexible and recyclable transient resistive memory device using bio-derived fish gelatin as the data storage media and dynamic covalent bonded polyimine networks as the recyclable substrate is proposed. [Display omitted] The recyclable, self-healing and easily-degradable transient electronic technology has aroused tremendous attention in flexible electronic products. However, integrating the above advantages into one single flexible electronic device is still a huge challenge. Herein, we demonstrate a flexible and recyclable bio-based memory device using fish colloid as the resistive switching layer on a polyimine substrate, which affords reliable mechanical and electrical properties under repetitive conformal deformation operation. This flexible bio-based memory device presents potential analog behaviors including memory characteristics and excitatory current response, which undergoes incremental potentiation in conductance under successive electrical pulses. Moreover, this device is expected to greatly alleviate the environmental problems caused by electronic waste. It can be decomposed rapidly in water and well recycled, which is a promising candidate for transient memories and information security. We believe that this study can provide new possibilities to the field of high-performance transient electronics and flexible resistive memory devices. [ABSTRACT FROM AUTHOR]

In this study, ultra-robust, nonfluorinated, and sub-zero temperature self-healing superhydrophobic coatings are fabricated by spray-coating imine-bond crosslinked polydimethylsiloxane-based supramolecular polymers (I-PDMS) and SiO 2 nanoparticles (NPs). Due to the synergy between I-PDMS binding and SiO 2 NPs reinforcement, the resulting I-PDMS/SiO 2 coatings can maintain their superhydrophobicity after sandpaper abrasion, sand impacting, hand tapping, and foot trampling and showed the best mechanical robustness among reported superhydrophobic coatings. Furthermore, due to the low glass-transition temperature of I-PDMS monomers and the dynamic nature of the imine bonds, the I-PDMS/SiO 2 coatings can spontaneously restore their damaged superhydrophobicity at − 30 °C through the free energy-driven diffusion of I-PDMS monomers. The I-PDMS/SiO 2 coatings can be used as friction layers for triboelectric nanogenerators (TENGs), which provide them with long-lasting waterproofing and self-cleaning capabilities, thus preventing their output performance from being degraded due to water infiltration and dust accumulation. Due to the excellent mechanical strength of the I-PDMS/SiO 2 coatings, the resulting self-healing superhydrophobic TENGs can generate electrical energy from repetitive motions such as hand tapping or foot trampling, which has not been possible in other reported superhydrophobic TENGs. [Display omitted] • Self-healing superhydrophobic coatings are prepared using supramolecular polymers. • The coatings are ultra-robust against various mechanical damages. • The coatings can spontaneously self-heal at sub-zero temperatures. • Self-healing superhydrophobic TENGs based on the coatings are obtained. • The TENGs can long-lasting harvest energy from human motions. [ABSTRACT FROM AUTHOR]

Gas-evolving electrodes often suffer from the blocking of catalytic active sites-due to unwanted and unavoidable adhesion of generated gas bubbles, which elevates the overpotential for the electrochemical hydrogen evolution reaction (HER)- by raising the resistance of the electrode. Here, a catalyst-free and self-healable superaerophobic coating having ultra-low bubble adhesion is introduced for achieving significantly depleted overpotentials of 209 and 506 mV at both low (50 mA cm -2 ) and high (500 mA cm -2 ) current densities, respectively, compared to a bare nickel-foam electrode. The optimized coating ensured an early detachment of the generated tiny (0.8 ± 0.1 mm) gas bubble-and thus, prevented the undesired rise in resistance of the coated electrode. The systematic association of physical (i.e., ionic interactions, H-bonding, etc.) cross-linkage, β-amino ester type covalent cross-linkage and reinforced halloysite nano clay enables the design of such functional material embedded with essential characteristics-including improved mechanical (toughness of 63.7 kJ m -3 , and tensile modulus of 26 kPa) property and chemical (extremes of pH (1 and 14), salinity, etc.) stability, rapid (<10 min) self-healing ability (even at alkaline condition) and desired bubble-wettability (bubble contact angle of 158.2 ± 0.2 ° ) with ultralow force (4.2 ± 0.4 µN) of bubble adhesion., (© 2024 Wiley‐VCH GmbH.)

Fluorescent elastomer materials have received extensive attention due to their excellent optical performance, flexibility, and chemical stability in recent years, and demonstrate great application potentials in intelligent sensors, optoelectronic devices, medical equipment and other fields. Although the traditional method for constructing fluorescent elastomers by doping fluorescent small molecules is facile and universal, it also has limitations such as low luminous efficiency, uneven dispersion, poor stability and single function. In this work, an aggregation-induced emission (AIE) fluorescent polymer with aldehyde groups in side chain was synthesized and crosslinked with aminopropyl double capped polydimethylsiloxane (NH 2 -PDMS-NH 2) through mild Schiff base reaction to construct a fluorescent elastomer. Compared with fluorescent small molecules, AIE polymers have superior fluorescence performance and can be flexibly designed according to demands. The dynamic imine bonds endow the as-obtained elastomers with self-healing and recycling properties, enabling rapid repair and remodeling at room temperature. Besides, the tensile and swelling properties of PDMS enable them to adjust the concentration of fluorescent units in the matrix under corresponding stimulus, thereby achieving tunable fluorescence emission. Taking advantage of the fluorescent elastomers, we prepared fluorescent anti-counterfeiting patterns that were hidden in daylight and visible under UV light, demonstrating the potential applications of the fluorescent elastomers in the fields of anti-counterfeiting and information encryption. This study also provides an alternative strategy for developing multifunctional fluorescent elastomers. This article reports the method of constructing fluorescent elastomer through dynamic imine bond using AIE polymer and NH 2 -PDMS-NH 2. The dynamic covalent bonds endow the as-obtained elastomer with self-healing and recycling properties. At the same time, the fluorescent elastomer also shows responsivity towards elongation and solvent. Finally, we took advantage of the fluorescent elastomer to prepare anti-counterfeiting patterns, exploring its potential applications in anti-counterfeiting and information encryption fields. [Display omitted] • AIE polymers with superior fluorescence properties are prepared. • The resulting fluorescent elastomers show responsivity towards elongation and solvent. • The fluorescent elastomers feature fast self-healing and recycling properties. • The elastomers hold potential applications in anti-counterfeiting and information encryption. [ABSTRACT FROM AUTHOR]

Learning about the strain/stress distribution in a material is essential to achieve its mechanical stability and proper functionality. Conventional techniques such as universal testing machines only apply to static samples with standardized geometry in laboratory environment. Soft mechanical sensors based on stretchable conductors, carbon-filled composites, or conductive gels possess better adaptability, but still face challenges from complicated fabrication process, dependence on extra readout device, and limited strain/stress mapping ability. Inspired by the camouflage mechanism of cuttlefish and chameleons, here an innovative responsive hydrogel containing light-scattering "mechano-iridophores" is developed. Force induced reversible phase separation manipulates the dynamic generation of mechano-iridophores, serving as optical indicators of local deformation. Patch-shaped mechanical sensors made from the responsive hydrogel feature fast response time (<0.4 s), high spatial resolution (≈100 µm), and wide dynamic ranges (e.g., 10-150% strain). The intrinsic adhesiveness and self-healing material capability of sensing patches also ensure their excellent applicability and robustness. This combination of chemical and optical properties allows strain/stress distributions in target samples to be directly identified by naked eyes or smartphone apps, which is not yet achieved. The great advantages above are ideal for developing the next-generation mechanical sensors toward material studies, damage diagnosis, risk prediction, and smart devices., (© 2023 Wiley-VCH GmbH.)

Self-healing is a new strategy for crack defect which is the main reason for the failure of composites. As an extrinsic self-healing system, the microvascular network system is capable of multiple healing cycles and rapid healing of large area damage. However, the embedment of micropipe network will affect the performance of matrix material. In this article, a microvascular network of self-healing material is optimized using non-dominated sorting genetic algorithm II. Two objective functions head loss and void volume fraction are considered. Finite element analysis and Hardy Cross iteration are performed to achieve the quantization of objective functions. One hundred sixty-five optimized solutions were obtained, and the void volume fraction was within the limits of [4.19%, 5.13%], whereas the head loss was within the limits of [9.63×10−7 m, 6.51×10−6 m]. According to the optimization results, the network was prepared and tested to validate the design and feasibility. The test result shows that the void volume fraction of the prepared network is 3.77%, lower than the designed value 4.43% which has a little effect on the matrix material. The network is interconnected and the healing agent can flow freely in it. The embedded network does not reduce the performance of epoxy resin. The optimization of microvascular network balances the mechanical properties and self-repairing properties of the matrix material. [ABSTRACT FROM AUTHOR]

A computational fracture analysis is conducted on a self‐healing particulate composite employing a finite element model of an actual microstructure. The key objective is to quantify the effects of the actual morphology and the fracture properties of the healing particles on the overall mechanical behaviour of the (MoSi2) particle‐dispersed Yttria Stabilised Zirconia (YSZ) composite. To simulate fracture, a cohesive zone approach is utilised whereby cohesive elements are embedded throughout the finite element mesh allowing for arbitrary crack initiation and propagation in the microstructure. The fracture behaviour in terms of the composite strength and the percentage of fractured particles is reported as a function of the mismatch in fracture properties between the healing particles and the matrix as well as a function of particle/matrix interface strength and fracture energy. The study can be used as a guiding tool for designing an extrinsic self‐healing material and understanding the effect of the healing particles on the overall mechanical properties of the material. [ABSTRACT FROM AUTHOR]

[Display omitted] • Electrochemical degradation of MnO 2 electrodes under OER. • Self-healing MnO 2 /polymeric composite activated by acidic pH. • MnO 2 /polymeric composite retains 70 % of capacitance after 10 OER. • Reversible and autonomous self-responsive mechanism for MnO 2 electrodes. In this study, we report the enhanced electrochemical performance of a MnO 2 electrode modified with a pH-sensitive co-polymer, activated at acidic pH, and designed to counteract MnO 2 degradation in aqueous aqueous pseudocapacitors. The conformation of this polymer is controlled by the local pH changes that occur at the electrode/electrolyte interface during electrochemical stress associated to oxygen evolution. As a proof of concept, we demonstrate that the addition of the pH-sensitive polymer contributes to improved electrode integrity and lifetime under over-polarization with oxygen evolution. After undergoing 10 cycles of electrochemical stress, the MnO 2 /pH-sensitive polymer composite retains ∼ 70 % of its capacitance. This remarkable result stands in stark contrast with the pristine MnO 2 electrode which fails catastrophically under the same stress conditions. We believe that this pH-induced self-protection mechanism represents a significant advancement in the development of novel smarter self-healing electroactive materials for the next generation of energy storage devices. [ABSTRACT FROM AUTHOR]

Lanthanide organometallic complexes exhibit strong luminescence characteristics, owing to their antenna effects. The f-d energy level transition causes this phenomenon, which occurs when ligands and the external electrons of lanthanide metals coordinate. Based on this phenomenon, we used two lanthanide metals, europium (Eu) and terbium (Tb), in the present study as the metal center for iminodiacetic acid ligands. Further, we developed the resulting fluorescent organometallic complex as a smart material. The ligand-metal bond in the material functioned as a metal chelating agent and a cross-linking agent in a dynamically coordinated form, thereby prompting the material to self-heal. Temperature-sensitive poly- N -isopropylacrylamide was incorporated into the material as the polymer backbone. Afterward, we combined it with water-soluble poly(vinyl alcohol) and an additional ligand from poly(acrylic acid) to fabricate a high-performance hydrogel composite material. The shrinkage and expansion of the polymer form a grid between the materials. Because of the different coordination stabilities of Eu 3+ and Tb 3+ , the corresponding material exhibits environmental responses toward excitation wavelength, temperature, and pH, thus generating different colors. When used in fabrics, the cross-linking mechanism of the material effectively looped the material between fabric fibers; furthermore, the temperature sensitivity of the polymer adjusted the size of pores between fabric fibers. At relatively higher temperatures (>32 °C), the polymer structure shrank, fiber pores expanded, and air permeability improved. Thus, this material appears to be promising for use in smart textiles.

A cohesive zone-based constitutive model, originally developed to model fracture, is extended to include a healing variable to simulate crack healing processes and thus recovery of mechanical properties. The proposed cohesive relation is a composite-type material model that accounts for the properties of both the original and the healing material, which are typically different. The constitutive model is designed to capture multiple healing events, which is relevant for self-healing materials that are capable of generating repeated healing. The model can be implemented in a finite element framework through the use of cohesive elements or the extended finite element method (XFEM). The resulting numerical framework is capable of modeling both extrinsic and intrinsic self-healing materials. Salient features of the model are demonstrated through various homogeneous deformations and healing processes followed by applications of the model to a self-healing material system based on embedded healing particles under non-homogeneous deformations. It is shown that the model is suitable for analyzing and optimizing existing self-healing materials or for designing new self-healing materials with improved lifetime characteristics based on multiple healing events. [ABSTRACT FROM AUTHOR]

A facile method based on sequential "water tolerant" cationic polymerization, followed by post-polymerization modification led to the synthesis of redox responsive and self-healing polystyrene- block -poly(2-thioethyl vinyl ether) diblock copolymer-based coating material. [Display omitted] • Synthesis of polystyrene- block -poly(2-chloroethyl vinyl ether) (PSt- b -PCEVE) diblock copolymers is achieved via sequential "water tolerant" cationic polymerization of St and CEVE. • The pendant -CH 2 CH 2 Cl functionalities of PSt- b -PCEVE diblock copolymers were selectively transformed to promising redox-responsive polystyrene- block -poly(2-thioethyl vinyl ether) (PSt- b -PTEVE) diblock copolymers. • The developed redox responsive material was employed for the construction of self-healing coating material. Poly(alkyl vinyl ether)-based functional copolymers have wide applications in many high-tech areas. However, their synthesis is still challenging which limits their applications. This article describes the synthesis of an unprecedented redox-responsive polystyrene- block -poly(2-thioethyl vinyl ether) (PSt- b -PTEVE) diblock copolymers via sequential "water tolerant" cationic polymerization of St and CEVE, followed by post-polymerization transformation of the pendant -CH 2 CH 2 Cl functionalities of PCEVE segment to -CH 2 CH 2 SH functionalities. The initiating system enabled controlled cationic polymerization of styrene (St), yielding well-defined PSt (at least up to 22500 g/mol) with relatively low dispersity (Đ ≤ 1.36) and polystyrene- block -poly(2-chloroethyl vinyl ether) (PSt- b -PCEVE) diblock copolymers with acceptable dispersity values (Đ ≤ 1.38) thereof, demonstrating high chain-end fidelity. The controlled character of the cationic polymerization reaction was confirmed by linear kinetic plots, linear increase of M n s (with low Đ s) and synthesis of PSts of changing M n s simply by varying initial [St] 0 /[Initiator] 0 feed ratio. The synthesized PSt- b -PTEVE diblock copolymers exhibited redox responsivity and self-healing behaviour. The self-healing property of the PSt- b -PTEVE diblock copolymer was studied by optical microscopy. For this, first, a mechanical cut was introduced in the cross-linked PSt- b -PTEVE thin films and then images were taken at regular intervals to investigate the healing. These promising PSt- b -PTEVE diblock copolymers might have potential applications in many emerging areas, including functional coating. [ABSTRACT FROM AUTHOR]