The strategy of using hybrid fillers with different geometric shapes and aspect ratios has been established to be an efficient way to achieve high-performance polymer composites. While, in spite of the recently renowned advances in this field, the mechanism of synergistic behavior in the system is still unclear and equivocal. In this study, we systematically investigated the mechanism for the synergistic reinforcement in an elastomer reinforced by nanocarbon hybrids consisting of 2D reduced graphene oxide (rGO) and 1D carbon nanotubes (CNTs). The improved dispersion state of hybrid filler was attested by Raman, UV-Vis spectra and morphological observations. In addition to the phenomenological evidences, we substantiated a stronger confinement effect of hybrid network on chain dynamics, for the first time, with molecular concepts by dielectric relaxation analysis. The formation of a glassy interphase with orders of magnitude slower chain dynamics than that for bulk chains has been explicitly demonstrated in the hybrid system. Besides improved dispersion upon hybridization, it is believed the formation of a glassy interphase is another crucial factor in governing the synergistic reinforcement capability of hybrid composites. We envision this new finding provides significant insight into the mechanism of synergistic behavior in hybrid-filled polymer composites with molecular concepts.

It remains a huge challenge to create advanced elastomers combining high strength and great toughness. Despite enhanced strength and stiffness, elastomeric nanocomposites suffer notably reduced extensibility and toughness. Here, inspired by the concept of sacrificial bonding associated with many natural materials, a novel interface strategy is proposed to fabricate elastomer/graphene nanocomposites by constructing a strong yet sacrificial interface. This interface is composed of pyridine-Zn2+-catechol coordination motifs, which is strong enough to ensure uniform graphene dispersion and efficient stress transfer from matrix to fillers. Moreover, they are sacrificial under external stress, which dissipates much energy and facilitates chain orientation. As a result, the strength, modulus, and toughness of the elastomeric composites are simultaneously strikingly enhanced relative to elastomeric bulk. This work suggests a promising methodology of designing advanced elastomers with exceptional mechanical properties by engineering sacrificial bonds into the interface.

Functional elastomer nanocomposites have found numerous applications in diverse hi-tech areas. Transport phenomena, such as electrical conductivity, thermal conductivity and gas/liquid barrier properties, have been the major focus of functional elastomer nanocomposite research. Despite essential progress in these areas, a summary and discussion of state-of-the-art strategies for regulating the transport performances of nanocomposites based on the transportation mechanisms of electrons, phonons and mass are lacking. In the present review, a brief introduction of transport mechanisms in elastomer nanocomposites precedes a systematic summary of the important progress in elastomer nanocomposites with electrical/thermal conductivities and lowered mass permeabilities, with emphasis on the latest structural control strategies for tuning transport properties. Key applications of functional elastomer nanocomposites related to transport phenomena are also introduced. Overall, this review summarizes the state of the art in the design and performance enhancement of elastomer nanocomposites based on the relationships between their structures and transport properties, governed by the components/composition, interface/dispersion and fabrication.

Reinforcing rubbers and expanding their application galleries are two important issues in material science and engineering. In this work, we demonstrate a bioinspired design of high-performance and macroscopically responsive diene-rubber by engineering sacrificial metal–ligand motifs into a chemically cross-linked architecture network. The metal–ligand bonds are formed through the coordination reaction between the pyridine groups in butadiene–styrene–vinylpyridine rubber (VPR) and metal ions. Under external load, the metal–ligand bonds serve as sacrificial bonds that preferentially rupture prior to the covalent network, which dissipates energy and facilitates rubber chain orientation. Based on the function mechanisms, the modulus, tensile strength, and toughness of the samples are simultaneously improved without sacrificing the extensibility, and these properties can be conveniently tuned by varying the structure parameters of the covalently cross-linked network and metal–ligand bonds. Moreover, the dissociation/re-formation of metal–ligand bonds upon heating/cooling can endow VPR with thermally triggered adaptive recovery for shape memory application.

The application of polymers as an essential class of material was greatly inhibited due to the aging failure of these versatile materials during normal use. Hence, it is generally recognized that stabilization against thermo-oxidative aging is indispensable to extend the service life of polymers for long-term applications. However, toxicity and pollution of the state-of-the-art antiaging technologies have long been puzzles in the polymer industry. Herein, sustainable carbon nanodots (CDs), synthesized by facile and cost-effective microwave-assisted pyrolysis, are used for first time as radical scavengers to resist the thermo-oxidative aging of elastomers. We have demonstrated that incorporation of the resultant CDs could be green and generic radical scavengers toward highly aging-resistant elastomers. Furthermore, by controlling the photoluminescent quantum yield of the CDs with various passivated agents, tunable radical scavenging activity was achieved. We established for the first time that the aging resistance originates from the prominent reactive radical scavenging activity of the CDs, which was rationally controlled by their photoluminescent quantum yield.