Experimental testing of the polymer–filler gel formation theory. II.

In Part I of the present article predictions of the polymer–filler gel formation theory were tested experimentally using fine-particle silica in natural rubber (NR) and in styrene–butadiene rubber (SBR). Part II brings a more detailed experiment–theory comparison using carbon blacks differing in specific surface area and structure, graphitized blacks, fume silica, and surface-modified (hydrophobized) fume silica. In the region of low and medium filler concentration c, the c-dependence of the fraction G of polymer in polymer–filler gel, of the fraction B of total filler-bound polymer, of the fraction w_disp of solvent-dispersed filler particles were found to be correctly predicted by the theory. The effect of filler characteristics and of the method of its incorporation into the polymer on the values of the adjustable parameters of the theory (filler surface adsorptivity, D, and filler particles connectivity, f) was determined and is discussed. In the region of very high c increasing positive deviations of D from the low-c behavior were observed and an explanation for this effect is proposed. © 1998 John Wiley & Sons, Inc. J Appl Polym Sci 69: 95–107, 1998     

Structure–property relationships of silica/silane formulations in natural rubber,isoprene rubber and styrene–butadiene rubber composites

The mechanical performance of natural rubber (NR), synthetic poly-isoprene rubber (IR), and styrene–butadiene rubber (SBR) composites filled with various silica/silane systems is investigated. The results are analyzed by referring to micro-mechanical material parameters, which quantify the morphological and structural properties of the polymer and filler network. These are obtained from fits with the dynamic flocculation model (DFM) describing the strongly nonlinear quasi-static stress–strain response of filler-reinforced elastomers as found from multihysteresis measurements of the investigated compounds. We focus on the reinforcement mechanisms of silica compounds with coupling and covering silane, respectively. The fitted material parameters give hints that the coupling silane provides a strong chemical polymer–filler coupling, which is accompanied by improved strength of filler–filler bonds for all three rubbers types. This may result also from the chemical coupling of short chains bridging adjacent silica particles. It implies larger stress values for the coupling silane and, in the case of NR and IR, a more pronounced “Payne effect” compared to the covering silane. In contrast, for SBR, the coupling silane delivers a lower Payne effect, which is explained by differences in the compatibility between rubber type and silane-grafted silica surface. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020 , 137, 48435.     

Kinetics of the phase selective localization of silica in rubber blends

The Fourier transformed infrared (FTIR) spectroscopy on the rubber‐filler gel has been used as a tool for the quantitative characterization of the phase selective silica localization in styrene butadiene rubber (SBR)/natural rubber (NR) blends. The so‐called rubber‐layer L was introduced to describe the selective wetting behavior of the rubber phases to the filler. SBR/NR blends filled with silica were the focus of the experimental investigation. NR shows a higher wetting rate than SBR. Silane addition does not affect the wetting of NR but slowdowns the wetting of SBR. With increasing chamber temperature the value of the rubber‐layer L of all mixtures increases owing to the different thermal activated rubber‐filler bonding processes. Using the wetting concept the kinetics of silica localization in the phases of heterogeneous rubber blends was characterized. Because of the higher wetting rate of the NR component, in the first stage of mixing of NR/SBR blends more silica is found in the NR phase than in the SBR phase. In the next stage, silica is transferred from the NR phase to the SBR phase until the loosely bonded components of NR rubber‐layer are fully replaced by SBR molecules. POLYM. COMPOS., 31:1701–1711, 2010. © 2010 Society of Plastics Engineers.     

Thermal and scanning electron microscopy/energy‐dispersive spectroscopy analysis of styrene–butadiene rubber–butadiene rubber/silicon dioxide and styrene–butadiene rubber–butadiene rubber/carbon black–silicon dioxide composites

Silica as a reinforcement filler for automotive tires is used to reduce the friction between precured treads and roads. This results in lower fuel consumption and reduced emissions of pollutant gases. In this work, the existing physical interactions between the filler and elastomer were analyzed through the extraction of the sol phase of styrene–butadiene rubber (SBR)–butadiene rubber (BR)/SiO₂ composites. The extraction of the sol phase from samples filled with carbon black was also studied. The activation energy (E_a) was calculated from differential thermogravimetry curves obtained during pyrolysis analysis. For the SBR–BR blend, E_a was 315 kJ/mol. The values obtained for the composites containing 20 and 30 parts of silica per hundred parts of rubber were 231 and 197 kJ/mol, respectively. These results indicated an increasing filler–filler interaction, instead of filler–polymer interactions, with respect to the more charged composite. A microscopic analysis with energy‐dispersive spectroscopy showed silica agglomerates and matched the decreasing E_a values for the SBR–BR/30SiO₂ composite well. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 96: 2273–2279, 2005     

Organomodified montmorillonite as filler in natural and synthetic rubber

The filler action of dodecylamine (12C) intercalated montmorillonite (MNT) referred to as organomodified montmorillonite (12C‐MNT) up to 4 wt % on natural rubber (NR) and styrene butadiene rubber (SBR) was studied and findings were compared with respect to the unmodified Na‐MNT. X‐ray analysis was used to calculate the interchain separation (R and R′), degree of crystallinity (X_c), and distortion factor (k). It is noted that R and R′ showed the opposite trend, whereas X_c as well as k showed overall increasing trend with an increasing amount of 12C‐MNT on both NR and SBR. For Na‐MNT (1 wt %) filled NR and SBR, the corresponding magnitude of R and R ′ and X_c showed nearly no change, whereas k_c increased significantly. The crosslinking density (v_c) does not show any significant changes in NR, whereas for SBR, it increases with increasing 12C‐MNT as filler. Interestingly, in the case of 1 wt % pure Na‐MNT used as filler for both NR and SBR, v_c was lower compared to the virgin rubbers. Both swelling index (s_i) and sol fraction (Q) do not show any significant variation for NR composites, whereas these decrease for SBR composites with increasing concentration of 12C‐MNT filler. On the contrary, NR and SBR with 1 wt % of Na‐MNT filler show greater magnitude of s_i and Q corresponding to the pure ones. Measurements of mechanical properties showed a significant increase in tensile strength and elongation at break for NR‐12C‐MNT (4 wt %) when compared with either virgin NR. In addition, modulus at the elongation at 100 and 200% in general increases with increasing loading of 12C‐MNT filler in NR. Similar observations were also noted in the case of SBR. Interestingly, when only pure Na‐MNT is used as filler, the strength of NR and SBR decreases drastically. Scanning electron microscopic studies were also to used support the mechanical behavior of NR‐12MNT and SBR‐12CMNT composites. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 92: 3583–3592, 2004     

Quantitative characterization of interfaces in rubber–rubber blends by means of modulated‐temperature DSC

Rubber–rubber blends are used widely in industry, for example, in tire manufacture. It is often difficult to characterize interfaces in such rubber–rubber blends quantitatively because of the similarity in the chemical structure of the component rubbers. Here, a new method was suggested for the measurement of the weight fraction of the interface in rubber–rubber blends using modulated‐temperature differential scanning calorimetry (M‐TDSC). Quantitative analysis using the differential of the heat capacity, dCp/dT, versus the temperature signal from M‐TDSC allows the weight fraction of the interface to be calculated. As examples, polybutadiene rubber (BR)–natural rubber (NR), BR–styrene‐co‐butadiene rubber (SBR), SBR–NR, and nitrile rubber (NBR)–NR blend systems were analyzed. The interfacial content in these blends was obtained. SBR is partially miscible with BR. The cis‐structure content in BR has an obvious effect on the extent of mixing in the SBR–BR blends. With increasing styrene content in the SBR in the SBR–BR blends, the interface content decreases. NR is partially miscible with both BR and SBR. The NBR used in this research is essentially immiscible with NR. The maximum amount of interface was found to be at the 50:50 blend composition in BR–NR, SBR–BR, and SBR–NR systems. Quantitative analysis of interfaces in these blend systems is reported for the first time. © 2000 John Wiley & Sons, Inc. J Appl Polym Sci 76: 1791–1798, 2000     

Dynamic mechanical properties of SBR and EPDM vulcanisates filled with cryogenically pulverized flexible polyurethane foam particles

The dynamic mechanical properties of rubber vulcanisates filled with cryogenically pulverized polyurethane foam particles, used as a reinforcing filler, were investigated with respect to storage modulus (E′), loss modulus, and the variation of glass transition temperature. Two rubbers were using styrene–butadiene rubber (SBR) and ethylene–propylene copolymer (EPDM). The effects of filler concentration and filler characteristics (such as particle size and moisture content) were also monitored. It was found that the optimum dynamic mechanical properties of the compounds were obtained when introducing the PU particles of 40–50 parts per hundred (pph) rubber in the SBR and 30 pph in the EPDM, the properties being affected by the size of PU particles and moisture content. © 1999 John Wiley & Sons, Inc. J Appl Polym Sci 74: 1129–1139, 1999     

Theory of bound rubber

A theory of bound rubber formation has been developed which treats the effect as random adsorption of structural units of polymer on reactive sites which are assumed to exist on the surface of filler particles. Equations are derived for the fraction of bound rubber and for the molecular weight distribution of free (unbound) rubber. The theory contains only one adjustable parameter, the filler surface area per reactive site, A₀. It is shown for the case of the Schulz distribution that the amount of bound rubber depends but slightly on the dispersion parameter of the polymer and is determined essentially by the adsorption index M?_w cP/A₀N_A, where c is the filler concentration, P is its specific surface area, and N_A is the Avogadro number. All of the experimentally observed features of the bound rubber effect, including preferential adsorption of large molecules, are correctly predicted, the quantitative agreement of the theoretical equations with available experimental data being satisfatory. This supports the underlying assumption that the processes involved in the polymer–filler interaction may be approximated by a random-process model.     

Fly ash particles and precipitated silica as fillers in rubbers. I. Untreated fillers in natural rubber and styrene–butadiene rubber compounds

In this study, we investigated the effects of untreated precipitated silica (PSi) and fly ash silica (FASi) as fillers on the properties of natural rubber (NR) and styrene–butadiene rubber (SBR) compounds. The cure characteristics and the final properties of the NR and SBR compounds were considered separately and comparatively with regard to the effect of the loading of the fillers, which ranged from 0 to 80 phr. In the NR system, the cure time and minimum and maximum torques of the NR compounds progressively increased at PSi loadings of 30–75 phr. A relatively low cure time and low viscosity of the NR compounds were achieved throughout the FASi loadings used. The vulcanizate properties of the FASi‐filled vulcanizates appeared to be very similar to those of the PSi‐filled vulcanizates at silica contents of 0–30 phr. Above these concentrations, the properties of the PSi‐filled vulcanizates improved, whereas those of the FASi‐filled compounds remained the same. In the SBR system, the changing trends of all of the properties of the filled SBR vulcanizates were very similar to those of the filled NR vulcanizates, except for the tensile and tear strengths. For a given rubber matrix and silica content, the discrepancies in the results between PSi and FASi were associated with filler–filler interactions, filler particle size, and the amount of nonrubber in the vulcanizates. With the effect of the FASi particles on the mechanical properties of the NR and SBR vulcanizates considered, we recommend fly ash particles as a filler in NR at silica concentrations of 0–30 phr but not in SBR systems, except when improvement in the tensile and tear properties is required. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 93: 2119–2130, 2004     

High-strain hysteresis of rubber vulcanizates over a range of compositions,rates, and temperatures

Hysteresis loss of natural rubber (NR) and styrene–butadiene rubber (SBR) vulcanizates having variations of loading of carbon black, silica, clay, resin, and curatives has been measured over a wide range of strain rates and temperatures as well as under swollen conditions. Hysteresis loss increases with an increase in strain rate, filler loading, resin loading (at high rates), crosslink density, and strain level. Hysteresis decreases with an increase in temperature, particle diameter of filler, and resin loading at high testing temperature. All the data of hysteresis loss of filled NR and SBR compounds have been found to be superimposable on single master curves with the help of the WLF shift factor. The master curves can be divided into three regions. The slope of the intermediate region, Δlog(hysteresis)/Δlog(Ra_T) has been found to be 0.1 for almost all the vulcanizates. Similar master plots have been obtained when the hysteresis loss has been measured at higher cycles and higher extensions and also by using the data of the hysteresis loss ratio. The hysteresis loss ratio of all the vulcanizates follows a similar trend, except for the highly crosslinked system, which shows a lower value. Carbon black contributes significantly to the hysteresis loss even when the energy dissipation is minimized by swelling. © 1997 John Wiley & Sons, Inc. J Appl Polym Sci 65: 1429–1439, 1997     

NH3-modified swelling of silica-filled silicone rubber

The NH₃-modified swelling method was used for fume silica-filled silicone rubber compounds and vulcanizates. The method provides an estimation of the polymer–filler interaction in the system. Bound rubber reduction due to the modified swelling is shown to be dependent on the silica surface silanol content in the compound. The swelling behavior of silica-filled vulcanizates was also studied in an NH₃ atmosphere. The fraction of polymer–filler attachments in the vulcanizates was found not to depend on the particle size of silica and its surface modification, depending only on the total polymer–filler contact area in the system. No relation was found between bound rubber content in a compound and swelling of a filled vulcanizate of the same composition. The strong rubber-to-filler adherence found in toluene changed to nonadherence under NH₃-modified swelling conditions. The NH₃-induced cleavage of silica–silicone rubber attachments was found to be nearly completely reversible. In the silica-filled silicone rubber vulcanizates, the fraction of polymer–filler attachments due to polymer–filler interaction represents a substantial contribution to the total number of network chains.     

Elastic Behaviour of Ternary Rubber-filled Vulcanizates

Near-equilibrium stress–strain measurements have been carried out on ternary rubber vulcanizates. The effect of variation of the butyl rubber content on the elastic behaviour of the ternary rubber vulcanizates has been studied. It has been found that butyl rubber (IIR) is less sensitive to the vulcanization system used than either natural rubber (NR) or styrene–butadiene rubber (SBR). One can obtain a partially crosslinked system with an IIR phase embedded in the crosslinked matrix of NR and SBR. The role played by carbon black during mixing of the ternary blend has been investigated. The Mooney–Rivlin relationship was used to describe the behaviour of the ternary rubber matrix. The constants 2C₁ and 2C₂ have been calculated by use of the strain-amplification factor and the total crosslink density of the ternary rubber–carbon black systems has been investigated. The data have been evaluated in terms of the molecular theories of rubber elasticity. The elastic behaviour was found to be intermediate between the affine and phantom limits of the theory. © of SCI.     

Electroactive alumina particles embedded in an acrylic elastomer

Composites of alumina particles embedded in a polar acrylic rubber polymer matrix are being investigated as potential electroactive polymer actuators. The measured FTIR spectra, XRD patterns, and SEM micrographs suggest that the alumina particles with an average diameter of 9.873 ± 0.034 μm having the rhombohedral form of the corundum phase are intercalated homogeneously within the acrylic rubber matrix. At an Al₂O₃ volume fraction of 0.144, the electrical conductivity increases from 10⁻⁹ to 10⁻⁸ (Ω m)⁻¹ at 500 Hz. The storage modulus without applied electrical field, G′_o, increases from 9,533 to 105,540 Pa, an order of—a single—magnitude increase, as the particle volume fraction is varied from 0 to 0.144. The increase in the matrix rigidity of the hybrid organic‐inorganic composites are because of the stress transfer from matrix to the reinforcement particles, the partial substitution of a soft matrix with a stiffer filler, and the segmental immobilization caused by the interaction between the matrix polymer chains and the filler surface. Under an applied electric field, induced dipole moments and particle‐particle interaction are generated, leading to an increase in the matrix rigidity. Under an applied electrical field, G′_{2 kV/mm} increases from 9,775 to 139,080 within the same volume fraction range, a difference of more than 30% is observed because of presence of an electrical field. POLYM. COMPOS., 2011. © 2010 Society of Plastics Engineers     

Effect of ultrasonic extrusion of star styrene-butadiene rubber on properties of carbon black- and silica-filled compounds and vulcanizates

Extrusion of star styrene-butadiene rubber (SBR) without and with ultrasonic treatment at amplitudes 3.5, 5, 7.5, and 10 μm was carried out. The molecular structure of untreated and treated star SBR was determined. Significant reduction of die pressure was observed during ultrasonic treatment due to the thixotropic and degradation effects. Ultrasonic treatment of star SBR at 3.5 μm created molecules of higher molecular weight via long-chain branching without gel formation. Ultrasonic treatment of star SBR at 5 μm created a small amount of gel. At high ultrasonic amplitudes more gel was generated hindering mixing of star SBR with silica. Extruded star SBR was compounded with carbon black and precipitated silica, with and without silane. It was found that the long-chain branching induced by ultrasonic treatment improved the rubber–filler interaction in precipitated silica without silane, as confirmed by the increase of bound rubber content. The filler–filler interaction was reduced in silica compounds without silane, as indicated by study of Payne effect. The significantly improved rubber–filler interaction and reduced filler–filler interaction led to an increase of the modulus at 100% elongation and tensile strength of SBR/silica vulcanizates. Extensive comparisons were made with earlier study on ultrasonic treatment of linear SBR. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 47451.     

Effect of fillers and additives on the properties of SBR vulcanizates

Methacrylic acid (MAA) and methyl methacrylate (MMA) were used as additives for peroxide‐cured styrene–butadiene rubber (SBR) filled with three inorganic fillers with different particle sizes and surface activity, for example, MgO, Mg(OH)₂, and BaSO₄. The experimental results show that the introduction of MAA can improve the mechanical properties of SBR vulcanizates filled with MgO, Mg(OH)₂, or BaSO₄. A small amount of MAA leads to significant increases in the modulus, tensile strength, and tear strength. MMA has little effect on the mechanical properties of the SBR vulcanizates. The SEM micrographs show that MAA can improve the interfacial bonding between SBR and the three kinds of fillers. The SBR–filler interaction was studied by Kraus plots. The relationship between the SBR–filler interaction and the mechanical properties was explored. m, a characteristic constant of a filler–SBR matrix, represents the interfacial bonding between fillers and SBR and the accumulated structure of the fillers. At a given ?, a high value of m means a strong interaction between SBR and the filler and, therefore, strong mechanical properties. The Payne effect of the SBR vulcanizates was observed, and the vulcanizates have low storage moduli at high strains and high storage moduli at low strains, and the moduli are nonlinear and increase the nonlinearity as the filler content increases. The loss moduli and loss factor reach their maximums at moderate and high strain amplitudes, respectively. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 88: 775–782, 2003     

Mechanical behavior of highly filled natural CaCO3 composites: Effect of particle size distribution and interface interactions

The mechanical behavior of poly(di‐methyl siloxane) (PDMS) composites containing high volume fractions of natural CaCO₃ particles of various particle size distributions was studied under tensile and oscillatory bending stresses, emphasizing the unique behavior of high filler loaded compositions. Composites containing the maximal possible solid loading of raw CaCO₃ were investigated for the effect of fatty acids surface treatment. The elastic modulus increased with increasing filler loading, following Chantler's model for dental composites when correlated with the absolute filler volume fraction. Good fit to “traditional” models, e.g., Frankle‐Acrivos and Halpin‐Tsai, was obtained by correlating the modulus values with the volume fraction relative to the maximal possible filler loading. A master curve of different particle size distributions and filler levels composites was obtained by using the relative volume fraction values, illustrating the effect of particle packing characteristics on small deformation mechanical behavior. A minor increase in T_g was found in parallel to the appearance of a T_m relaxation peak at approximately −40°C. A peak temperature shift at T_m and a pronounced increase in this peak with increasing filler fraction was found as well. The changes in the melting transition are attributed to the constraints of the filler particles acting on the crosslinked melting polymer. Surface treatment with fatty acids significantly degraded the tensile properties. Interestingly, an increase of 4 vol% filler was enabled owing to the surface treatment, while restoring reasonable tensile properties. No significant effect was observed for excess of fatty acids resulting from physically adsorbed acids. Tan δ curves reveal low PDMS‐CaCO₃ particles interactions, and mobility of the PDMS chains in the increased filler fraction as in the treated 64 vol% composite, both higher than those in the raw composite. POLYM. COMPOS., 2008. © 2008 Society of Plastics Engineers     

Effect of carbon‐based nanoparticles on the cure characteristics and network structure of styrene–butadiene rubber vulcanizate

The network structure of styrene–butadiene rubber (SBR) in the presence of carbon black (CB) with two different structures and multi‐walled carbon nanotubes (MWCNTs) was investigated. Swelling behaviour, tensile properties at various strain rates and cure kinetics were characterized. Experimental data were analysed using the Flory–Rehner model as well as the tube model theory. It is found that the network structure of CB‐filled SBR follows a three‐phase composite model including rigid particles, semi‐rigid bound rubber and matrix rubber. This bound rubber is postulated to be critical for the mechanical and deformational properties, development of crosslinking density in matrix rubber and polymer–filler interaction. For MWCNT‐filled SBR, the bound rubber does not show a substantial contribution to the network structure and mechanical performance, and these properties are greatly dominated by the higher aspect ratio and polymer–filler interaction. Additionally it is deduced that the crosslinking density of matrix rubber increases on incorporation of the fillers compared to unfilled matrix rubber. Copyright © 2012 Society of Chemical Industry     

Selective wetting and dispersion of filler in rubber composites under influence of processing and curing additives

The present work highlighted the effect of commonly used processing and curing additives on the wetting and dispersion kinetics of filler like silica and carbon black (CB) in some examples using the methods like the wetting concept and online measured electrical conductance. The adsorption of additives and mono-functional silane on silica surface increases the wetting speed of silica in single compound of nitrile butadiene rubber (NBR), natural rubber (NR) and styrene butadiene rubber (SBR) compounds. In rubber blend, for instance NBR/NR, the extent of filler surface fraction wetted by each blend component is strongly dependent on the additive/silica and silane/silica ratio r. A model based on the surface tension data of rubber components and filler (Z-model) was used for prediction of the selective filler wetting at a thermodynamic equilibrium state. By combining the experimental results from the wetting concept and theoretical prediction from the Z-model the silica surface tension changed during mixing can be characterized. It quantitatively describes the deactivation of the silanol groups on the silica surface by adsorbed additives. The effect of adsorption of additives on filler dispersion was exemplarily demonstrated on CB filled SBR compounds by means of the method of online measured electrical conductance. The influence of additives on the CB dispersion in low styrene-content SBR mixtures is much more pronounced than that in high styrene-content SBR mixtures.     

Use of natural rubber prophylactics waste as a potential filler in styrene–butadiene rubber compounds

Owing to the unstable nature of the latex compound and the strict specifications in the quality of latex products such as condoms and examination gloves, the rejection in the latex industry comes to about 10 to 15% of the rubber consumed. These latex rejects contain about 95% rubber hydrocarbon of very high quality. A cost-effective technique has been developed for the reuse of natural rubber (NR) prophylacties waste in styrene–butadiene rubber (SBR). The influence of powdered latex rejects on the curing characteristics, mechanical properties, and failure behavior of SBR has been investigated. More emphasis is placed on the effect of both particle size and the loading of latex waste filler. Swelling studies were carried out to establish the degree of crosslinking of SBR and to assess the extent of interaction between the matrix and latex waste filler of varying particle sizes. A three layer model has been set up to study the diffusion of sulfur from the matrix phase to the filler phase. Scanning electron microscopy has been used to analyze the particle morphology, filler dispersion, and filler-matrix interface adhesion. The results of the study revealed that NR prophylactics rejects can be used effectively as a potential filler in SBR up to about 40 phr loading. © 1996 John Wiley & Sons, Inc.     

Effects of modified silica on the co-vulcanization kinetics and mechanical performances of natural rubber/styrene–butadiene rubber blends

Rubber blends are widely used for combining the advantages of each rubber component. However, to date, how to determine and distinguish the vulcanization kinetics for each single rubber phase in rubber blends during the co-vulcanization process is still a challenge. Herein, high-resolution pyrolysis gas chromatography–mass spectrometry (HR PyGC-MS) was employed for the first time to investigate the vulcanization kinetics of natural rubber (NR) and styrene–butadiene rubber (SBR) in NR/SBR blends filled with modified silica (SiO₂). The reaction rates of crosslinking of each rubber phase in NR/SBR were calculated, which showed that the crosslinking rates of NR were much lower than those of SBR phase in the unfilled blends and blends filled with unmodified and silane modified silica. Interestingly, the vulcanization rates of NR and SBR phase were approximately same in the vulcanization accelerator modified silica filled blends, showing better co-vulcanization. In addition, the vulcanization accelerator modified silica was uniformly dispersed and endowed rubber blends with higher mechanical strength compared to the untreated silica. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020 , 137, 48838.