Nanocomposites with polymer matrix provide tremendous opportunities to investigate new functions beyond those of traditional materials. The global community is gradually tending toward the use of composite and nanocomposite materials. This review is aimed at reporting the recent developments and understanding revolving around hybridizing fillers for composite materials. The influence of various analyses, characterizations, and mechanical properties of the hybrid filler are considered. The introduction of hybrid fillers to polymer matrices enhances the macro and micro properties of the composites and nanocomposites resulting from the synergistic interactions between the hybrid fillers and the polymers. In this review, the synergistic impact of using hybrid fillers in the production of developing composite and nanocomposite materials is highlighted. The use of hybrid fillers offers a viable way to improve the mechanical, thermal, and electrical properties of these sophisticated materials. This study explains the many tactics and methodologies used to install hybrid fillers into composite and nanocomposite matrices by conducting a thorough analysis of recent research. Furthermore, the synergistic interactions of several types of fillers, including organic-inorganic, nano-micro, and bio-based fillers, are fully investigated. The performance benefits obtained from the synergistic combination of various fillers are examined, as well as their prospective applications in a variety of disciplines. Furthermore, the difficulties and opportunities related to the use of hybrid fillers are critically reviewed, presenting perspectives on future research paths in this rapidly expanding area of materials science.

In recent years, conductive polymer nanocomposites have gained significant attention due to their promising thermoresistive and Joule heating properties across a range of versatile applications, such as heating elements, smart materials, and thermistors. This paper presents an investigation of semi-crystalline polyvinylidene fluoride (PVDF) nanocomposites with 6 wt.% carbon-based nanofillers, namely graphene nanoplatelets (GNPs), multi-walled carbon nanotubes (MWCNTs), and a combination of GNPs and MWCNTs (hybrid). The influence of the mono- and hybrid fillers on the crystalline structure was analyzed by X-ray diffraction (XRD) and differential scanning calorimetry (DSC). It was found that the nanocomposites had increased amorphous fraction compared to the neat PVDF. Furthermore, nanocomposites enhanced the β phase of the PVDF by up to 12% mainly due to the presence of MWCNTs. The resistive properties of the nanocompositions were weakly affected by the temperature in the analyzed temperature range of 25-100 °C; nevertheless, the hybrid filler composites were proven to be more sensitive than the monofiller ones. The Joule heating effect was observed when 8 and 10 V were applied, and the compositions reached a self-regulating effect at around 100-150 s. In general, the inclusion in PVDF of nanofillers such as GNPs and MWCNTs, and especially their hybrid combinations, may be successfully used for tuning the self-regulated Joule heating properties of the nanocomposites.

Investigating biodegradable and biocompatible materials for electronic applications can lead to tangible outcomes such as developing green-electronic devices and reducing the amount of e-waste. The proposed emulsion-based conducting ink formulation takes into consideration circular economy and green principles throughout the entire process, from the selection of materials to the production process. The ink is formulated using the biopolymer polylactic acid dissolved in a sustainable solvent mixed with water, along with conductive carbon nanotubes (CNTs) and silver flakes as fillers. Hybrid conductive fillers can lower the percolation threshold of the ink and the production costs, while maintaining excellent electrical properties. The coating formed after the deposition of the ink, undergoes isothermal treatment at different temperatures and durations to improve its adhesion and electrical properties. The coating\'s performance was evaluated by creating an eight-finger interdigitated sensor using a Voltera PCB printer. The sensor demonstrates exceptional performance when exposed to various loading and unloading pressures within the 0.2-500.0 kPa range. The results show a consistent correlation between the change in electrical resistance and the stress caused by the applied load. The ink is biodegradable in marine environments, which helps avoiding its accumulation in the ecosystem over time.

Graphene and its derivatives have been confirmed to be among the best fillers for rubber due to their excellent properties, such as high mechanical strength, improved interface interaction, and strain-induced crystallization capabilities. Graphene rubber materials can be widely used in tires, shoes, high-barrier conductive seals, electromagnetic shielding seals, shock absorbers, etc. In order to reduce the graphene loading and endow more desirable functions to rubber materials, graphene-based hybrid fillers are extensively employed, which can effectively enhance the performance of rubber composites. This review briefly summarizes the recent research on rubber composites with graphene-based hybrid fillers consisting of carbon black, silica, carbon nanotubes, metal oxide, and one-dimensional nanowires. The preparation methods, performance improvements, and applications of different graphene-based hybrid fillers/rubber composites have been investigated. This study also focuses on methods that can ensure the effectiveness of graphene hybrid fillers in reinforcing rubber composites. Furthermore, the enhanced mechanism of graphene- and graphene derivative-based hybrid fillers in rubber composites is investigated to provide a foundation for future studies.

The synergistic effect between different fillers plays a crucial role in determining the performance of composites. In this work, spherical boron nitride (BN) and flaky BN are used as hybrid fillers to improve the thermal conductivity (TC) of high-density polyethylene (HDPE) composites. A series of HDPE composites were prepared by adjusting the mass ratio (1:0, 4:1, 2:1, 1:1, 1:2, 1:4, and 0:1) of spherical BN and flaky BN. The SEM results indicate that the spherical BN (with a particle size of 3 μm) effectively filled the gaps between the flaky BN (with a particle size of 30 μm), leading to the formation of more continuous heat conduction paths with the composite. Remarkably, when the mass ratio of spherical BN to flaky BN was set to 1:4 (with a total BN filling amount of 30 wt%), the TC of the composite could reach up to 1.648 Wm-1K-1, which is obviously higher than that of the composite containing a single filler, realizing the synergistic effect of the hybrid fillers. In addition, the synergistic effect of fillers also affects the thermal stability and crystallization behavior of composites. This work is of great significance for optimizing the application of hybrid BN fillers in the field of thermal management.

The development of thermally conductive rubber nanocomposites for heat management poses a formidable challenge in numerous applications, notably within the realm of tire technology. Notably, rubber materials are characterized by their inherently low thermal conductivity. Consequently, it becomes imperative to incorporate diverse conductive fillers to mitigate the propensity for heat build-up. Multi-walled carbon nanotubes (MWCNTs), as reinforcement agents within the tire tread compounds, have gained considerable attention owing to their extraordinary attributes. The attainment of high-performance rubber nanocomposites hinges significantly on the uniform distribution of MWCNT. This study presents the influence of MWCNTs on the performance of carbon black (CB)-reinforced natural rubber (NR)/styrene butadiene rubber (SBR) tire compounds prepared via high shear melt mixing. Morphological analysis showed a good distribution of MWCNTs in the NR/SBR/CB compound. The vulcanization parameters, such as the maximum and minimum torque, cross-linking density, hardness, abrasion resistance, tensile strength, and Young modulus, exhibited a progressive improvement with the addition of MWCNT. Remarkably, adding MWCNT into CB improved the heat conductivity of the NR/SBR/CB compounds, hence decreasing the heat build-up. A percolation mode was also proposed for the hybrid carbon fillers based on the data obtained.

The limited ionic conductivity at room temperature and the constrained electrochemical window of poly(ethylene oxide) (PEO) pose significant obstacles that hinder its broader utilization in high-energy-density lithium metal batteries. The garnet-type material Li6.4 La3 Zr1.4 Ta0.6 O12 (LLZTO) is recognized as a highly promising active filler for enhancing the performance of PEO-based solid polymer electrolytes (SPEs). However, its performance is still limited by its high interfacial resistance. In this study, a novel hybrid filler-designed SPE is employed to achieve excellent electrochemical performance for both the lithium metal anode and the LiFePO4 cathode. The solid composite membrane containing hybrid fillers achieves a maximum ionic conductivity of 1.9 × 10-4 S cm-1 and a Li+ transference number of 0.67 at 40 °C, respectively. Additionally, the Li/Li symmetric cells demonstrate a smooth and stable process for 2000 h at a current density of 0.1 mA cm-2 . Furthermore, the LiFePO4 /Li battery delivers a high-rate capacity of 159.2 mAh g-1 at 1 C, along with a capacity retention of 95.2% after 400 cycles. These results validate that employing a composite of both active and inactive fillers is an effective strategy for achieving superior performance in all-solid-state lithium metal batteries (ASSLMBs).

Thermally conductive polymeric composites are promising for heat management in microelectronic devices. This work presents a binary-hybrid composite of boron nitride (BN) nanoparticles and micro-diamond (D) fillers in an elastomeric polyurethane (PU) matrix which can be three- dimensionally printed to produce a highly flexible and self-supporting structure. The research shows that a combination of 16.7 wt% BN and 16.7 wt% D results in a robust network within the polymer matrix to improve the tensile modulus more than nine times with respect to neat PU. Significantly, the hybrid matrix enhances the thermal conductivity by more than two times when compared to neat PU. The enhancement in mechanical, and thermal features make this three-dimensional printable multiscale hybrid composite suitable for flexible and stretchable microelectronic applications.

We studied the effects of silicon carbide (SiC) and SiC hybrid systems with different conventional fillers (silica, carbon black, graphene, hydrotalcite, halloysite) on the rheometric measurements, crosslink density, mechanical performance, aging stability, morphology, thermal behaviour, and flammability of ethylene-propylene-diene (EPDM) rubber composites. The hybrid filler systems showed technically promising synergetic effects on the performance of the EPDM composites. A pronounced reinforcing effect in EPDM composites filled with hybrid SiC filler systems was noted. Tensile strength increased in the systems with carbon black, silica, and graphene nanoplatelets, by 21%, 37%, and 68%, respectively, compared to the neat EPDM. Dynamic-mechanical analysis (DMA) revealed a shift of the glass transition temperature (Tg) of EPDM composites towards higher values following the incorporation of hybrid SiC fillers, indicating that the mobility of the macromolecule chains was restricted by the presence of filler particles. Importantly, the application of SiC as a filler in EPDM rubber composites contributed to a considerable reduction in flammability, as demonstrated by microscale combustion calorimetry (MCC). The most promising results were obtained for HAL/SiC and LDH/SiC hybrid systems, which produced final composites with high flame retardancy and good mechanical performance. The study highlights the significant potential of SiC and SiC hybrid systems as effective fillers improving the properties of elastomer composites.

Multifunctional structural materials are very promising in the field of engineering. Particularly, their strain sensing ability draws much attention for structural health monitoring applications. Generally, strain sensing materials are produced by adding a certain amount of conductive fillers, around the so-called \"percolation threshold\", to the cement or composite matrix. Recently, graphite has been found to be a suitable filler for strain sensing. However, graphite requires high amounts of doping to reach percolation threshold. In order to decrease the amount of inclusions, this paper proposes cementitious materials doped with new hybrid carbon inclusions, i.e., graphite and carbon microfibers. Carbon microfibers having higher aspect ratio than graphite accelerate the percolation threshold of the graphite particles without incurring into dispersion issues. The resistivity and strain sensitivity of different fibers\' compositions are investigated. The electromechanical tests reveal that, when combined, carbon microfibers and graphite hybrid fillers reach to percolation faster and exhibit higher gauge factors and enhanced linearity.