Healable and Recyclable Elastomers with Record‐High Mechanical Robustness, Unprecedented Crack Tolerance, and Superhigh Elastic Restorability

Abstract

Spider silk is one of the most robust natural materials, which has extremely high strength in combination with great toughness and good elasticity. Inspired by spider silk but beyond it, a healable and recyclable supramolecular elastomer, possessing superhigh true stress at break (1.21 GPa) and ultrahigh toughness (390.2 MJ m−3), which are, respectively, comparable to and ≈2.4 times higher than those of typical spider silk, is developed. The elastomer has the highest tensile strength (ultimate engineering stress, 75.6 MPa) ever recorded for polymeric elastomers, rendering it the strongest and toughest healable elastomer thus far. The hyper‐robust elastomer exhibits superb crack tolerance with unprecedentedly high fracture energy (215.2 kJ m−2) that even exceeds that of metals and alloys, and superhigh elastic restorability allowing dimensional recovery from elongation over 12 times. These extraordinary mechanical performances mainly originate from the meticulously engineered hydrogen‐bonding segments, consisting of multiple acylsemicarbazide and urethane moieties linked with flexible alicyclic hexatomic spacers. Such hydrogen‐bonding segments, incorporated between extensible polymer chains, aggregate to form geometrically confined hydrogen‐bond arrays resembling those in spider silk. The hydrogen‐bond arrays act as firm but reversible crosslinks and sacrificial bonds for enormous energy dissipation, conferring exceptional mechanical robustness, healability, and recyclability on the elastomer.

Ultrastretchable and Stable Conductive Elastomer Based on Micro-Ionicgel for Wide-Working-Range Sensors

“…In the next few cycles, IL-CE 80 exhibited excellent fatigue durability, in which the stress–strain curves were almost overlapped. Notably, the maximum stress and the energy loss coefficient were maintained at 68.3 and 59.3%, respectively, without a sustained and noticeable decrease (Figure e). , To further demonstrate the excellent toughness of the elastomers, puncture resistance tests were performed by puncturing the samples with a needle (inset of Figure f) Figure f shows the force–displacement curves of the elastomers with diverse vinyl-SiO 2 nanoparticle contents, from which an obvious increase of force was observed on increasing the vinyl-SiO 2 nanoparticle contents.…”

Interface Chelation Induced by Pyridine‐Based Polymer for Efficient and Durable Air‐Processed Perovskite Solar Cells

“…[16] Significantly,the formation of hydrogen bonding was also verified in Figure S10 and was summarized in Table S1. [17] Moreover,the obvious shifts of Pb 4f 7/2 and 4f 5/2 peaks also verified the strong interaction between SHP and Pb 2+ . [4b] Besides,a saconsequence of the incorporation of SHP additive,t he binding energy of I3 d 3/ 2 and 3d 5/2 became smaller than that without SHP,i ndicating ah igh electronegativity in Figure 3d.…”

Organic Single‐Crystal Actuators and Waveguides that Operate at Low Temperatures

“…The polymers used included thermoplastic polyether urethanes (TPU), styrene−butadiene−styrene block copolymer (SBS), and poly(vinyl chloride) (PVC) which were procured from commercial sources, and poly(urethane urea) elastomer (IPDI-SPU) which was prepared in this work. [31] Poly(diallyldimethylammonium) (PDDA) and poly(styrenesulfonate) (PSS) were first alternatively deposited on the surface of 1-3 by using the layer-by-layer self-assembly method. [32] These surface-modified crystals were then coated with poly(vinyl alcohol) (PVA) to protect them from dissolution.…”

“…The change in slope at −67.1 °C clearly corresponds to the glass transition temperature (T g ) of IPDI-SPU. [31] The elastomer is rigid below, but it becomes more flexible above this temperature, and this affects the stiffness of the actuator. Correspondingly, the linear correlation slope from −67.1 to −17.2 °C is greater than that of −115.5 to −67.1 °C.…”