Elastomer Matrix Research Articles

Bidirectional Zero Poisson's Ratio Elastomers with Self‐Deformable Soft Mechanical Metamaterials for Stretchable Displays

AbstractStretchable displays, capable of reversible expansion, represent significant advancements in free‐form display technologies. However, the high Poisson's ratio (ν) of elastomer substrates leads to unintended deformation under tensile strain, resulting in image warping. To address this, a meta‐elastomer (ME) substrate with a bidirectional zero ν, incorporating a self‐deformable soft mechanical metamaterial (MM) frame, is introduced. The ν of the ME is precisely programmed by the interaction between the deformation of the MM frame, which exhibits a negative ν, and the elastomer matrix, which has a positive ν. The soft MM frame, stiffer than the elastomer matrix, undergoes both structural deformation and length alteration during substrate tensile strain. This synergistic effect enables achieving a nearly bidirectional zero ν, thus overcoming the limitations of conventional tessellated rigid MM composites. Furthermore, the ME substrate, which is chemically cross‐linked at the junction interface, demonstrates exceptional mechanical robustness, enduring over 180% stretching and more than 10 000 cycles. By counteracting the Poisson's effect, the ME substrate with an integrated pixel array ensures translational pixel movement along the tensile axis during bidirectional stretching, minimizing undesired pixel movement in other directions. The stretchable ME presents key advancements for implementing more stable and reliable stretchable display applications.

Experimental dynamic thermal properties determination of EPDM/NBR panels with a shape stabilized Phase Change Material based on summer daily temperatures of four cities in Italy

In this work, the evaluation of E-PCM panels based on an elastomeric matrix containing a shape-stabilized paraffinic phase change material with a melting point of 28 °C was carried in a climatic chamber, simulating the summer daily temperature profile of four geographical locations in Italy at different latitudes. The characterization, carried out on testing boxes insulated using the E-PCM panels, allowed the determination of the delay (time lag) and of the dampening (decrement factor) in the propagation of the heat wave when passing from the outer to the inner surface of the walls; the results were correlated to two important parameters, the characteristic admittance and the heat capacity. From the difference between the heat fluxes on the outer and inner surface of the panels it was also possible to quantify the amount of stored energy and to do a comparison with a reference insulating panel (aerogel). Aerogel panels, despite the low thermal conductivity but due to the limited heat capacity and characteristic admittance, were unable to provide an effective insulation during summer conditions while E-PCM panels led to excellent outcomes. Results showed that with a peak of 33 °C in the external temperature, the phase change material limited the internal one at 27 °C with a maximum delay in the peak temperature of 6 h, an overall decrement factor of 0.4, time lag of 3 h and stored energy of 740 kJ/m2 per day. Finally, also the influence of the testing speed on the response of the E-PCM was evaluated through repetition of heating/cooling cycles in the temperature range 19–35 °C, highlighting the necessity of improving the thermal conductivity of the system in case of fast-response applications (cycle length < 3.5 h) and/or to optimize the PCM amount in the panel depending on the energy to be absorbed.

Enhancement of controllable circular actuator using graphene oxide particles

ABSTRACT This work aims to study the responsive expansion of graphene oxide- acrylic elastomer (GO-Acry ER elastomer) under applied electric field. The GO was synthesized from graphite (GP) by using Hummer’s method based on various the ratios of GP to oxidizing agent namely potassium permanganate. GO-Acry ER elastomer was prepared by painted GO as the polarized particle on circular Acry ER as elastomer matrix. The optimum condition of synthesized GO was 1:2 ratios of GP: oxidizing agent which provided a more crystallinity, smaller particle size, and higher pore volume. The circular actuation response of GO-Acry ER elastomer was stimulated by applying external stimuli under various electric field strengths and GO characteristics. The expansion of the GO-Acry ER elastomer increased with an increasing external electric field strength. The GO-Acry ER elastomer under adding GO of 1:2 ratios was the largest expansion with 50% strain under applied electric field of 300 kV/mm. When the electric field strength was > 300 kV/mm, the ER elastomer shrank owing to electrical breakdown. Thus, GO is a suitable choice due to its ease of preparation and fast electro-responsive properties.

3D Printing of Customizable Transient Bioelectronics and Sensors

AbstractTransient electronics have emerged as a new category of devices that can degrade after their functional lifetime, offering tremendous potential as disposable sensors, actuators, wearables, and implants. Additive manufacturing methods represent a promising approach for patterning transient materials, yet examples of fully printed bioelectronic devices are scarce. This study introduces a fully digital 3D printing approach enabling the prototyping and customization of soft bioelectronics made of transient materials. The direct ink writing of poly(octamethylene maleate (anhydride) citrate) (POMaC) as an elastomeric matrix and of a shellac‐carbon ink as a conductor is investigated. Precise and repeatable deposition of both structural and conductive features is achieved by optimizing printing parameters, i.e., the dispense gap, printing speed, and inlet pressure. Multi‐material 3D printing enables the fabrication of functional transient devices. Notably, pressure and strain sensors are shown to operate in ranges relevant to implanted biomechanical monitoring. 3D‐printed transient electrodes are demonstrated to be comparable to state‐of‐the‐art devices in terms of impedance behavior. Finally, physical degradation of the materials is confirmed at physiological conditions. These fully digital additive manufacturing processes enable the monolithic fabrication of customizable transient bioelectronics with adaptable functions and geometries.

Chameleon-inspired tunable multi-layered infrared-modulating system via stretchable liquid metal microdroplets in elastomer film

This report presents liquid metal-based infrared-modulating materials and systems with multiple modes to regulate the infrared reflection. Inspired by the brightness adjustment in chameleon skin, shape-morphing liquid metal droplets in silicone elastomer (Ecoflex) matrix are used to resemble the dispersed “melanophores”. In the system, Ecoflex acts as hormone to drive the deformation of liquid metal droplets. Both total and specular reflectance-based infrared camouflage are achieved. Typically, the total and specular reflectances show change of ~44.8% and 61.2%, respectively, which are among the highest values reported for infrared camouflage. Programmable infrared encoding/decoding is explored by adjusting the concentration of liquid metal and applying areal strains. By introducing alloys with different melting points, temperature-dependent infrared painting/writing can be achieved. Furthermore, the multi-layered structure of infrared-modulating system is designed, where the liquid metal-based infrared modulating materials are integrated with an evaporated metallic film for enhanced performance of such system.

Magnetic polyurethane based composites as contactless valves in microfluidic applications

Magnetoactive polymer composites have garnered significant attention for their potential use in diverse applications, owing to their rapid and reversible response to external magnetic fields. By incorporating magnetic nanoparticles (MNPs) into an elastomeric matrix, these composites exhibit unique properties under static or alternating magnetic fields. In this context, thermo-polyurethane-based magnetic active composites are promising materials for developing microfluidic system components such as valves and peristaltic pumps. In the current study, we investigated the utilization of cobalt ferrite (CoFe2O4) magnetic nanoparticles in conjunction with a non-toxic synthesis method for polyurethane. It was explored the impact, on the overall success of the process, of cobalt ferrite nanoparticles incorporation at various stages of the thermo-polyurethane (TPU) synthesis reaction. Finally, the effects of different amounts of MNPs on the physicochemical properties of the resulting composites and their behavior as actuators under the influence of a magnetic field, was investigated. Our studies reveal that the actuator response of the composites increases proportionally with the percentage of MNPs present.Finally, the performance of a TPU/7.5% (V/V) CoFe2O4 composite strip as a flow control actuator within a microfluidic system was evaluated. This actuator responds to magnetic fields by bending, resulting in a 10% reduction in flow rate of microfluidic system. Reversing the magnetic field restores the flow rate to its initial value. Our cyclic tests illustrate the actuator's capacity to locally and temporarily modulate the microfluidic system's resistance. When combined with tailored TPU elasticity, these materials show significant potential for the fabrication of microfluidic valves and pumps.

Compliant composite elastomers via grafting short dangling chains for promoting thermal transport performance

AbstractThe multifunctional composite elastomers serve as thermal interface materials for heat dissipation in electronic devices when their thermal transport performance is enhanced. The common method for enhancement, continuously raising the thermal conductive filler loading only can improve thermal conductivity of composite elastomers but reduces compliance, resulting in elevated contact thermal resistance with solid surfaces, compromising thermal transport. To address this, we propose grafting short dangling chains onto the composite elastomer matrix to further promote compliance under a certain filler loading. Characterization results demonstrate that the grafted chains effectively reduce relaxation time, enabling faster deformation for the material under pressure. This approach enhances interfacial compatibility, widening the thermal transport path at contact interfaces to contact thermal resistance by 94% (from 17.8 to 1.07 mm2W/K), significantly improving overall thermal transport. Additionally, we discussed the feasibility of employing composite elastomers as thermal interface materials for efficient chip heat dissipation.Highlight The grafted dangling chains can promote the composite elastomers softness. The softness promotion can help reduce thermal contact resistance. A series of theories are employed to learn the mechanisms of the promotion. The resulting composite elastomers can be used as thermal interface materials.

Ionic Liquid Enabled Transparent Heterogeneous Elastomers for Soft Electronics

AbstractDielectric elastomer (DE), as an electrically active soft material, has enabled stretchable electronics, electronic skins, artificial muscles, biomimetic soft robots, and non‐magnetic motors. High permittivity is urgently desired for increasing the sensitivity of DE sensors and lowering the driving voltage of DE actuators. However, existing efforts for significantly enhanced permittivity is usually achieved at the expense of transparency of the DE by compositing external fillers, which limits the applications in optoelectronics, such as displays, touch screens, artificial eyes, etc. Here, by utilizing of transparent functional filler, ionic liquid micro‐droplet, and precise matching the refractive index with polydimethylsiloxane (PDMS) elastomer matrix, heterogeneous composites with high transparency and high permittivity are obtained simultaneously. The composites are transparent in the visible range (transmittance, 80%–95%). The permittivity reaches up to 22, which is more than seven times higher than the original value of the elastomer matrix. Moreover, the arbitrary deformability of ionic liquid filler endows the composites with better stretchability (300%) and much lower elastic modulus (0.5 MPa, about a quarter the value of PDMS), which is beneficial for soft electronics. Based on the as‐prepared high‐performance composites, high sensitivity and transparent soft sensors and touch panels have been realized, as well as wireless transmission of sensing signals.

93‐1: Invited Paper: Meta‐Elastomer for Biaxially Stretchable Displays Without Image Distortion

Stretchable displays are garnering attention due to their ability to undergo reversible shape deformation. However, due to Poisson's ratio, image distortion issues caused by undesired substrate deformations during stretching remain challenging. Here, we propose meta‐elastomers with biaxially zero Poisson's ratio for distortion‐free stretchable displays. To program the Poisson's ratio according to biaxial stretching, elastomeric mechanical metamaterial (MM) frames with a negative Poisson's ratio are integrated into an elastomer matrix. By leveraging competitive interactions between the elastomeric MM frame and elastomer matrix deformation, we have successfully implemented the biaxial near‐zero Poisson's ratio substrates.

Highly flexible and transparent self-healing elastomer based on localized supramolecular interactions with enhanced mechanical properties and long-term storage stability

This study prepared a highly flexible and transparent self-healing elastomer with enhanced mechanical properties and long-term storage stability, facilitated by localized supramolecular interactions. By incorporating a functional oligomer containing localized urea groups into a conventional elastomeric matrix, increased supramolecular interactions were promoted through multiple hydrogen bonds among clustered functional groups. The resulting supramolecular elastomers exhibited excellent optical properties, including total transmittance exceeding 90 %, yellow index less than 2, and haze under 1 %, along with elastic recovery of 40 %. Notably, the self-healing elastomer developed in this study effectively overcame the typical trade-off between mechanical and self-healing properties in conventional self-healing materials, achieving superior mechanical strengths compared to conventional elastomers and an outstanding self-healing efficiency of 94.0 % within a few minutes. Moreover, by tailoring the chemical structure of the oligomer, significant improvements in the long-term solution storage stability of the solution for urea systems were achieved. These results are attributed to the unique supramolecular network derived from multiple hydrogen bonding interactions among the localized functional groups in a confined zone. A mechanism for improved mechanical properties and outstanding self-healing performance is also proposed using a model system.

Modelling the magnetic-mechanical coupled viscoelastic behaviour of transversely isotropic soft magnetorheological elastomers

Soft magnetorheological elastomers (s-MRE) is a kind of smart material mainly fabricated by embedding soft magnetic particles into an elastomer matrix. It can be categorized as isotropic and transversely isotropic, depending on the arrangement of internal magnetic particles. In isotropic s-MRE, magnetic particles are randomly distributed, while transversely isotropic s-MRE forms chain structures for the magnetic particles. Compared with isotropic s-MRE, transversely isotropic s-MRE exhibits more significant magnetically-enhanced mechanical properties, making it highly applicable in the vibration control area. While past theoretical work has mainly focused on the magneto-mechanical coupling behaviour of isotropic s-MRE, less attention has been given to modelling the magneto-mechanical coupling behaviour of transversely isotropic s-MRE. Specifically, understanding the impact of different particle chain-magnetic field spatial locations on the magnetization and magnetic-enhanced viscoelastic behaviour of transversely isotropic s-MRE remains an open topic. To address this research gap, we characterize the quasi-static, viscoelastic and magnetization performance of transversely isotropic s-MRE under different particle chain-magnetic field spatial locations. Subsequently, we develop a novel constitutive model for transversely isotropic s-MRE, integrating magneto-hyperelasticity, magneto-viscoelasticity and magnetization. We then implement the magneto-mechanical coupled model for transversely isotropic s-MRE at a finite element level. Following model calibration and validation, we conduct a case study to demonstrate the model’s ability to predict the magneto-mechanical coupling performance of a transversely isotropic s-MRE-based laminated isolator. This model is a valuable tool for predicting the magneto-mechanical performance of transversely isotropic s-MRE-based smart devices, thereby facilitating the design and advancement of transversely isotropic s-MRE in vibration control.

Epoxy modified styrene butadiene rubber (SBR) in green tire application

Styrene butadiene rubber (SBR) is an important elastomer in tire application. The tire industries are facing challenges in optimizing the magic triangle, which balances three contradicting properties: abrasion resistance, wet traction, and rolling resistance (RR). There are numerous approaches foroptimizingtire compound characteristics, which eventually impact tire performance. Choosing an appropriate kind of reinforcing filler is one of the techniques that may be used. Silica based tires give better traction properties and low rolling resistance, but silica has hydroxyl groups on the surface, and it is not compatible with non-polar elastomers such as Emulsion-based Styrene Butadiene Rubber (ESBR). Hence, it is necessary to incorporate some polar moieties into ESBR chains to enhance the compatibility with silica. In this study, non-polar Emulsion-based Styrene Butadiene Rubber (ESBR) is transformed into polar ESBR by modifying with epoxidizing reagent at room temperature. The epoxidized-ESBR (E-ESBR) was characterized by 1H NMR, FT-IR, and DSC analyses. Synthesized E-ESBR was compounded with ESBR and silica filler for the ‘green tire’ tread compounding (ESBR-Silica/E-ESBR). The incorporation of E-ESBR improved silica dispersion in the ESBR matrix. Hence, the tensile strength of ESBR-Silica/E-ESBR compound improved. The rolling resistance decreased compared to the ESBR-Silica compound. Furthermore, dry, wet, and snow traction properties of the compounded system were improved by 9 %, 25 %, and 37 %, respectively, in comparison to the pristine EBSR-Silica compound. Thus, the incorporation of the E-ESBR system could generate a new pave for better dispersion of silica in the non-polar elastomer matrix.

Stretchable Metal Halide Perovskite Color Conversion Layers with Block Copolymer Dispersant

AbstractStretchable luminescent nanocomposites with metal halide perovskite (MHP) emitters are in high demand as deformable color‐conversion layers (CCLs) for vivid‐colored form‐factor free displays. However, the immiscibility of the MHP crystals with an elastomeric polymer matrix induces particle aggregation with resultant luminescence quenching, hindering the development of MHP‐based CCLs. Herein, a simple method is proposed to produce highly luminescent MHP nanoparticles (NPs) and stably disperse them in an elastomeric poly(dimethylsiloxane) (PDMS) polymer matrix with block copolymer (BCP) dispersant. The nanocomposites are developed through sequential steps of synthesis of MHP‐NP dispersion solution with BCP and blending with PDMS followed by thermal curing. It is revealed that Lewis basic poly(2‐vinylpyridine)‐block‐poly(dimethylsiloxane) (P2VP‐b‐PDMS) BCP added in the synthesis step promotes crystallization of the MHPs as nanocrystals with an average diameter of 5.9 ± 1.2 nm, whereas MHPs with hundreds of nm are produced without BCP. The resultant MHP‐NPs with P2VP‐b‐PDMS exhibit excellent photophysical properties, such as narrow band emission, high photoluminescence (PL) quantum yield, and long PL lifetime. The MHP‐NPs are stably dispersed in the PDMS matrix by P2VP‐b‐PDMS without particle aggregation, leading to highly deformable and stretchable nanocomposites with stable PL emission upon repetitive stretching, and excellent environmental stability.

In-situ graft fibrous PPy@PEI enables sensitive and all-seasoned crack monitoring for ancient architectures based on flexible pressure sensors

The non-destructive, real-time, and automatic monitoring for the development of cracks in ancient architectures is crucial to the preservation of precious ancient heritages. Here, light-weight crack sensing constructed with ultra-thin and high-performance flexible pressure sensors is proposed to fulfill this demand. The signal drift and poor reversibility commonly observed in widely-reported sensors based on elastomer matrix, which originates from the creep and relaxation behaviors, are addressed using piezoresistive polypyrrole-grafted polyetherimide fibers. The corresponding flexible piezoresistive sensors exhibit great sensitivity (9.45 kPa−1 in 0 ∼ 1 kPa and 3.48 kPa−1 in 3 ∼ 10 kPa), outstanding static stability (5.13 % signal drift after 48 h under 1 kPa), dynamic durability (4.72 % degradation after ∼30,000 cycles) and excellent robustness across an ultra-wide temperature range of −70 ∼ 150 ℃. Based on this highly reliable pressure sensor, the proposed non-destructive crack sensors integrated into an Internet of Things (IoT) platform display outstanding stability during their service in the Forbidden City. By virtue of the low energy consumption, one lithium battery can power the monitoring system for more than one year.

Mechanical Properties Comparison of Isotropic vs. Anisotropic Hybrid Magnetorheological Elastomer-Fluid.

Magnetorheological (MR) materials are smart materials that can change their rheological characteristics when exposed to a magnetic field. Such rheological properties include viscosity and dynamic modulus. MR materials have emerged as one of the most efficient smart materials that can modify mechanical and viscoelastic characteristics. Depending on the medium used, MR materials can be classified into two types: magnetorheological fluids (MRFs) and magnetorheological elastomers (MREs). MREs are classified as isotropic or anisotropic based on CIP distribution inside the elastomer matrix. A unique hybrid material incorporating MRE and MRF is constructed in this work to investigate, compare, and the dynamic properties of isotropic, anisotropic, hybrid isotropic, and hybrid anisotropic MREs under various magnetic fields (0, 104, and 160.2 mT). The created samples are subjected to extensive testing, including static and dynamic evaluations. In the static tests, experiments use a compression linear displacement mode with a fixed maximum gap change of 3 mm. The temperature is maintained at a constant level of 24 °C throughout the 40 s test duration for each test, and the magnetic field is incrementally increased by varying the number of magnets, ranging from 0 to 160.2 mT for dynamic qualities using compression oscillations on a dynamic mechanical analyzer (DMA), including frequency and strain-dependent data. These experiments, carried out using sinusoidal shear movements, include an excitation frequency range of 0.1 Hz to 15 Hz while preserving, with a fixed shear strain of 2%.

Effect of Modified and Unmodified Oak Bark (Quercus Cortex) on the Cross-Linking Process and Mechanical, Anti-Aging, and Hydrophobic Properties of Biocomposites Produced from Natural Rubber (NR).

The study explores the novel use of oak bark (Quercus cortex) as a bio-filler in elastomeric composites, aligning with the global trend of plant-based biocomposites. Both modified and unmodified oak bark were investigated for their impact on the physicochemical properties of natural rubber (NR) composites. The bio-filler modified with n-octadecyltrimethoxysilane exhibited enhanced dispersion and reduced aggregates in the elastomeric matrix. NR composites containing more than 20 phr of unmodified and modified oak bark demonstrated an increased degree of cross-linking (αc > 0.21). Mechanical properties were optimal at 10-15 phr of oak bark and the sample with modified bio-filler (10 phr) achieved the highest tensile strength (15.8 MPa). Silanization and the addition of the bio-filler increased the hardness of vulcanizates. The incorporation of oak bark improved aging resistance at least two-fold due to phenolic derivatives with antioxidant properties. Hydrophobicity decreased with added bark, but silanization reversed the trend, making samples with a high content of oak bark the most hydrophobic (contact angle: 129°). Overall, oak bark shows promise as an eco-friendly, anti-aging filler in elastomeric composites, with modification enhancing compatibility and hydrophobicity.

Discrete-to-continuum modeling of spider silk fiber composites

This work presents a discrete-to-continuum approach to the constitutive response of composite materials formed by embedding a network of spider silk fibers in a matrix material. A multiscale model that makes use of the virial stress concept of statistical mechanics is formulated, which accounts for hyperelastic constitutive equations of the component materials. The finite element implementation of the given constitutive equations is also carried out. Numerical simulations show the response of a silk composite formed by embedding a spider orb web in a matrix material, and illustrate the main features of the proposed model. In the presence of a weak matrix, the force–displacement response of a silk composite is compared with that deriving from an atomistic modeling of the spider orb web. A simulation of the response of a composite equipped with an elastomeric matrix is also discussed.

Highly Transparent and Long‐Term Stable Dielectric Elastomer Composites Enabled by Poly(ionic liquid) Inclusion

AbstractThe demand for high‐performance flexible electronic devices has propelled research toward dielectric elastomer composites that exhibit excellent stretchability, high dielectric constant, exceptional transparency, and enduring stability. Compositing with soft fillers is an emerging method that can increase the dielectric constant of the materials while retaining good flexibility. However, liquid metals inclusion results in opaque composites while liquid electrolytes inclusion brings issues with long‐term stability. In this study, compositing polymeric ionic liquids with elastomeric matrix is proposed to address these requisites. Benefiting from adjustable refractive index, high ionic conductivity, softness, and excellent stability, the prepared dielectric elastomer composites exhibit remarkable transparency, excellent elasticity, and increased dielectric constants. Notably, the composites demonstrate resilience to high temperatures up to 250 °C without compromising dielectric or mechanical properties. Furthermore, the composites retain all properties after prolonged exposure at 80 °C for 6 months, highlighting the potential for sustained performance in real‐world applications. Utilizing the exceptional characteristics of polymeric ionic liquid including dielectric elastomers, strain sensors, and alternating current electroluminescence devices are demonstrated, which also presents excellent stability over prolonged use, emphasizing the reliability and long‐term stability of the composites, and showcasing potentials for multifaceted applications in flexible electronics.

Unraveling Morphology and Chemistry Dynamics in Fluoroethylene Carbonate Generated Silicon Anode Solid Electrolyte Interphase Across Delithiated and Lithiated States: Relative Cycling Stability Enabled by an Elastomeric Polymer Matrix

The silicon solid electrolyte interphase (SEI) faces cyclical cracking and reconstruction due to the ∼350% volume expansion. Understanding the SEI dynamic morphology and chemistry evolution from delithiated to lithiated states is thereby paramount to engineering a stable Si anode. Fluoroethylene carbonate (FEC) is a preferred additive with widely demonstrated enhancement of the Si cycling. Thus, insights into the dynamics of the FEC-SEI may provide hints toward engineering the Si interface. Herein, complementary ATR-FTIR, AFM, tip IR, and XPS probing reveal the presence of an elastomeric polycarbonate-like matrix in the FEC-generated SEI which is absent from the FEC-free SEI. Adding FEC to the baseline 1 M LiPF6 in EC:EMC (1:1) electrolyte promotes formation of a thinner and more conformal SEI, and subdues morphology and chemistry changes between consecutive half-cycles. From AFM, morphological stabilization of the FEC-SEI occurs earlier. Furthermore, conventional SEI biproducts such as Li2CO3 and LiEDC appear in reduced quantities in the FEC-SEI implying a reduced quantity of Li-consuming species. The thin polymeric FEC-SEI enables deeper (de)lithiation of silicon. In conclusion, the enhanced mechanical compliance, chemical invariance, and reduced Li inventory consumption of the FEC-SEI are logically the key features underlying the Si cycling enhancement by FEC.

Tea Grounds as a Waste Biofiller for Natural Rubber.

The aim of this study was the utilization of ground tea waste (GT) left after brewing black tea as a biofiller in natural rubber (NR) composites. Ionic liquids (ILs), i.e., 1-ethyl-3-methylimidazolium lactate and 1-benzyl-3-methylimidazolium chloride, often used to extract phytochemicals from tea, were applied to improve the dispersibility of GT particles in the elastomeric matrix. The influence of GT loading and ILs on curing characteristics, crosslink density, mechanical properties, thermal stability and resistance of NR composites to thermo-oxidative aging was investigated. The amount of GT did not significantly affect curing characteristics and crosslink density of NR composites, but had serious impact on tensile properties. Applying 10 phr of GT improved the tensile strength by 40% compared to unfilled NR. Further increasing GT content worsened the tensile strength due to the agglomeration of biofiller in the elastomer matrix. ILs significantly improved the dispersion of GT particles in the elastomer and increased the crosslink density by 20% compared to the benchmark. Owing to the poor thermal stability of pure GT, it reduced the thermal stability of vulcanizates compared to unfilled NR. Above all, GT-filled NR exhibited enhanced resistance to thermo-oxidation since the aging factor increased by 25% compared to the unfilled vulcanizate.