Cure Characteristics and Mechanical Properties of Vinyltriethoxysilane Grafted Styrene-Butadiene Rubber/Silica Blends

Graft polymerization of vinyltriethoxysilane (VTES) onto styrene-butadiene rubber (SBR) was carried out in latex using potassium peroxydisulfate as an initiator. Then SBR-g-VTES/silica, SBR/TESPT/silica and SBR-g-VTES/TESPT/silica were prepared by mechanical mixing with different silica loading. The silica particles dispersed uniformly in the SBR-g-VTES networks. Among the three composites, the SBR-g-VTES/Silica blends show the highest of all. The t₉₀ of SBR-g-VTES/TESPT/Silica composites is the shortest of all. On the other hand, the SBR-g-VTES/TESPT/silica composites exhibit highest tensile strength and hardness of all. The SBR-g-VTES/silica composites show higher tensile strength and hardness than SBR/TESPT/silica. The tanδ value (loss tangent) at ?20-0°C of SBR-g-VTES/silica is slightly higher than that of SBR/TESPT/silica.     

Reinforcing effect of silica on the properties of styrene butadiene rubber–reclaim rubber blend system

Incorporation of silica into styrene butadiene rubber (SBR)–reclaim rubber (RR) blend system was carried out by sol–gel technique and conventional method. A well known silica coupling agent bis(3‐triethoxysilyl propyl) tetrasulfide was found to affect the curing characteristics and mechanical properties of SBR/RR vulcanizate. Here, the effect of RR on silica reinforcement was studied for different SBR/RR blend system. Silica incorporation by conventional mechanical mixing in absence of TESPT showed a much higher tensile properties than that of silica incorporated by the in situ sol–gel reaction of tetraethoxy silane both in presence and absence of TESPT. Studies of equilibrium swelling in a hydrocarbon solvent were also carried out. ATR study indicates that RR forms bond with silica particles due to the presence of active functional site on RR. The amount of silica incorporated by sol–gel reaction was determined through thermogravimetric analysis (TGA). Scanning electron microscopy (SEM) studies further indicate the coherency and homogeneity in the silica filled SBR/RR vulcanizate. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 99: 957–968, 2006     

Reinforcement of peroxide‐cured styrene–butadiene rubber vulcanizates by mathacrylic acid and magnesium oxide

Through the neutralization of magnesium oxide (MgO) and methacrylic acid (MAA), magnesium methacrylate [Mg(MAA)₂] was in situ prepared in styrene–butadiene rubber (SBR) and used to reinforce the SBR vulcanizates cured by dicumyl peroxide (DCP). The experimental results show that the mechanical properties, dynamic mechanical properties, optical properties, and crosslink structure of the Mg(MAA)₂‐reinforced SBR vulcanizates depend on the DCP content, Mg(MAA)₂ content, and the mole ratio of MgO/MAA. The formulation containing DCP 0.6–0.9 phr, Mg(MAA)₂ 30–40 phr, and MgO/MAA mole ratio 0.50–0.75 is recommended for good mechanical properties of the SBR vulcanizates. The tensile strength of the SBR vulcanizates is up to 31.4 MPa when the DCP content is 0.6 phr and the Mg(MAA)₂ content is 30 phr. The SBR vulcanizate have good aging resistance and limited retention of tensile strength at 100°C. The SBR vulcanizates are semitransparent, and have a good combination of high hardness, high tensile strength, and elongation at break. The T_g values of the SBR vulcanizates depend largely on the DCP content, but depend less on the Mg(MAA)₂ content and the MgO/MAA mole ratio. The contents of DCP, Mg(MAA)₂, and the MgO/MAA mole ratio have also great effects on the E′ values of the vulcanizates. The salt crosslink density is greatly affected by the Mg(MAA)₂ content and MgO/MAA mole ratio, but less affected by the DCP content. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 85: 2667–2676, 2002     

Regulation of trans‐1,4‐polyisoprene crystallinity and mechanical properties of styrene‐butadiene rubber/trans‐1,4‐polyisoprene vulcanizate

The effects of processing temperature and bis‐[γ‐(triethoxysilyl)‐propyl]‐tetrasulfide (Si69) on crystallization, morphology, and mechanical properties of styrene‐butadiene rubber (SBR)/trans‐1,4‐polyisoprene (TPI) vulcanizate are investigated. The crystallinity and crystalline melting temperature (T_m) of TPI in the vulcanizates with TPI/silica/(Si69) pre‐mixed at 150 °C are much lower than that pre‐mixed at 80 °C. At the same pre‐mixing temperature, the presence of 1 phr Si69 leads to a decreased crystallinity and T_m. The TPI domains with phase size of about 1 μm and silica are well dispersed in the vulcanizate, and TPI crystals get smaller in size and less in amount by pre‐mixing TPI, silica and Si69 at 150 °C. The vulcanizates with TPI/silica/(Si69) pre‐mixed at 150 °C have decreased tensile strength and modulus at a given extension than that pre‐mixed at 80 °C. At the same pre‐mixing temperature, the tensile strength and modulus of the vulcanizate increase with the addition of 1 phr Si69. The crystallinity of TPI component in SBR/TPI vulcanizate is effectively controlled by changing processing temperature and adding Si69, which is important for theoretical research and practical application of TPI. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 44395.     

Mechanical and dynamic mechanical properties of natural rubber blended with waste rubber powder modified by both microwave and sol–gel method

Waste rubber powder (WRP) was modified by microwave, sol–gel method, and both microwave and sol–gel method, respectively. The mechanical and dynamic mechanical properties of natural rubber (NR)/modified WRP composite were investigated. The influence of bis‐(3‐(triethoxysilyl)‐propyl)‐tetrasulfide (TESPT) content on curing characteristics and mechanical properties of vulcanizate was also studied. The results showed that NR/WRP modified by both microwave and sol–gel method composite owned the best mechanical properties. Rubber processing analyzer was used to characterize the interaction between silica and rubber chains and the dispersion of silica. With increase of TESPT content, the Payne effect decreased. Scanning electron microscopy indicated the coherency and homogeneity of in situ generated silica filled vulcanizate. Dynamic mechanical analyzer showed that NR/WRP modified by both microwave and sol–gel method composite with 5 phr TESPT exhibited the lower tan δ at temperature range of 50–80°C, compared with composite without TESPT and the higher tan δ at temperature of 0°C, compared with the conventional modification of WRP. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

The Effect of Electron Beam (EB) Irradiation in Presence of TMPTA on Cure Characteristics and Mechanical Properties of Styrene Butadiene Rubber/Recycled Acrylonitrile-Butadiene Rubber (SBR/NBRr) Blends

The effect of electron beam (EB) irradiation on the cure characteristics and mechanical properties of unirradiated and irradiated SBR/NBRr blends were investigated. The SBR/NBRr blends were prepared at 95/5, 85/15, 75/25, 65/35, and 50/50 blend ratio with and without the presence of a polyfunctional monomer, trimethylolpropane triacrylate (TMPTA). Results indicated that the scorch time t₂, cure time t₉₀ and minimum torque (M_L) of irradiated SBR/NBRr blend decreased, but the maximum torque (M_H) particularly at 35 and 50 phr of NBRr (recycled NBR) increased with the presence of TMPTA. The stress at 100% elongation (M100), hardness, cross-linking density and tensile strength (particularly after 15 phr of NBRr content) of irradiated SBR/NBRr blends increased after irradiation but the elongation at break (EB) and resilience decreased. The irradiated SBR/NBRr blends showed lower thermal stability than non-irradiated blends. Scanning electron microscopy proved the enhancement in tensile strength when more NBRr were added in SBR matrix where the irradiated surfaces demonstrate more irregularity with increasing crack branching (fracture planes are located at different heights) due to the increased of cross-linked density.     

Curing Characteristics and Mechanical and Morphological Properties of Styrene Butadiene Rubber/Virgin Acrylonitrile-Butadiene Rubber (SBR/vNBR) and Styrene Butadiene Rubber/Recycled Acrylonitrile-Butadiene Rubber (SBR/rNBR) Blends

Curing characteristics and mechanical and morphological properties of styrene butadiene rubber/virgin acrylonitrile-butadiene rubber (SBR/vNBR) and styrene butadiene rubber/recycled acrylonitrile-butadiene rubber (SBR/rNBR) were investigated. Results indicated that the curing characteristics, such as scorch time, t₂, and cure time, t₉₀, of SBR/vNBR and SBR/rNBR blends decreased with increasing vNBR and rNBR content. At similar blend ratios, particularly up to 15 phr, SBR/rNBR blends exhibited higher t₂ and t₉₀ compared with SBR/vNBR blends. Minimum torque (ML) and maximum torque (MH) of SBR/vNBR blends significantly increased with increasing vNBR content. For SBR/rNBR blends, ML increased with increasing rNBR content, but MH exhibited the opposite trend. Tensile strength, elongation at break (E_b), resilience, and fatigue decreased with increasing virgin and recycled NBR content in both blends. Up to 15 phr, the tensile strength, E_b and fatigue life (Kc) of SBR/rNBR blends were higher than in SBR/vNBR blends. The M100 (stress at 100% elongation), hardness, and cross-linking density of both blends also showed an increasing trend with increasing vNBR and rNBR content. The scanning electron microscopy study indicates that rNBR exhibited a weak rNBR-SBR matrix interaction particularly when more than 15 phr of rNBR was used, thus decreasing the mechanical properties of SBR/rNBR blends.     

Estimation of silica flocculation in SBR/BR compounds reinforced with different silica contents from their rheocurves

The rheocurves of silica-filled styrene–butadiene/polybutadiene rubber (SBR/BR) compounds containing 3-octadecyltriethoxy silane (OTES) and bis-[triethoxysilylpropyl]tetrasulfide (TESPT) were investigated to examine the effects of silica content and silanes on silica flocculation during mixing and cure. SBR/BR compounds without curatives were also prepared to infer the effect of cure on silica flocculation. The maximum torque of the compounds could be deconvoluted to individual source torques such as silica flocculation during mixing and cure, crosslinking of rubber, and coupling between rubber and silica by assuming the independence of silica flocculation from cure and coupling. Torque due to silica flocculation increased with the silica content of the SBR/BR compounds, but its effect was significantly reduced by the addition of OTES or TESPT. TESPT suppressed silica flocculation and facilitated coupling, thus yielding enhanced tensile properties. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020 , 137, 48559.     

Effect of thermal exposure on the microstructure and strength of an alumina-silica ceramic fiber

The microstructure and mechanical properties of an alumina-silica ceramic fiber after thermal exposure at 1100–1300°C were investigated by X-ray diffraction, nuclear magnetic resonance, scanning electron microscopy, transmission electron microscopy analyses and room temperature tensile strength test. The results showed that the fiber was composed of γ-A1₂O₃ and amorphous SiO₂. A phase reaction of γ-A1₂O₃ and amorphous SiO₂ occurred when thermal exposure temperature exceeded 1150°C, and a new mullite phase formed. The grain size of the newly formed mullite increased with the increase of exposure temperature. Both the phase transition and grain growth of mullite had a significant impact on the mechanical properties of the fiber. Tensile strength of the fiber decreased slightly when thermal exposure temperature was below 1150°C, while the strength retention of the fiber decreased sharply to 65.36% as exposure temperature rose to 1200°C. A higher dispersion of tensile strength was also observed at higher exposure temperatures, as revealed by the Weibull statistical model.     

Effect of triblock copolymers on homogeneity,mechanical properties and swelling behavior of IIR/SBR rubber blends

The present research concerns with the preparation and characterization of isobutylene isoprene/butadiene–styrene rubber (IIR/SBR) blends with different blend ratios, in the presence and absence of styrene–isoprene–styrene (SIS) and styrene–isobutylene–styrene (SiBS) triblock copolymers to be tested as compatibilizers. Effect of the triblock copolymers on the blend homogeneity was investigated with the aid of scanning electron microscopy (SEM) and differential scanning calorimetry (DSC) measurements. Characterization of the rubber blends was conducted by measuring the physico-mechanical properties after and before thermal aging, in presence and absence of the triblock copolymers. In addition, weight swell % in toluene, motor oil and brake fluid of the rubber blend vulcanizates was assessed. The incorporation of SIS and SiBS triblock copolymers improved the homogeneity of IIR/SBR blends as well as increased both tensile strength and elongation at break of the rubber blend vulcanizates. Of the entire blend ratios examined, IIR/SBR (25/75) blend containing SIS compatibilizer possessed the best physico-mechanical properties (12.6 MPa tensile strength and 425 % elongation at break) and (14 MPa tensile strength and 555 % elongation at break) after and before thermal aging, respectively. Utilization of SIS and SiBS triblock copolymers enhanced the thermal stability of IIR/SBR blend vulcanizates. Moreover, IIR/SBR blends of different blend ratios showed superior swelling resistance in the brake fluid. IIR/SBR (25/75) blend containing SIS compatibilizer and cured with CBS/ZDEC/S vulcanizing system possessed the best physico-mechanical properties (14.4 MPa tensile strength and 440 % elongation at break) and (16.5 MPa tensile strength and 610 % elongation at break) after and before thermal aging, respectively.     

High-temperature mechanical properties of NextelTM 610 fiber reinforced silica matrix composites

Novel Nextel? 610 fiber reinforced silica (N610f/SiO₂) composites were fabricated via sol-gel process at a sintering temperature range of 800–1200?°C. The sintering-temperature dependent microstructures and mechanical properties of the N610f/SiO₂ composites were investigated comprehensively by X-ray diffraction, nanoindentation, three-point bending etc. The results suggested a thermally stable Nextel? 610 fiber whose properties were barely degraded after the harsh sol-gel process. A phase transition in the silica matrix was observed at a critical sintering temperature of 1200?°C, which led to a significant increase in the Young's modulus and hardness. Due to the weak fiber/matrix interfacial interaction, the 800?°C and 1000?°C fabricated N610f/SiO₂ composites exhibited quasi-ductile fracture behaviors. Specially, the latter possessed the highest flexural strength of ≈ 164.5?MPa among current SiO₂-matrix composites reinforced by fibers. The higher sintering-temperature at 1200?°C intensified the SiO₂ matrix, but strengthened the interface, thus resulting in a brittle fracture behavior of the N610f/SiO₂ composite. Finally, the mechanical properties of this novel composite presented good thermal stability at high temperatures up to 1000?°C.     

One-step synthesis of improved silica/epoxy nanocomposites with inorganic-organic hybrid network

High performance silica/epoxy nanocomposites were prepared through mixing epoxy, tetraethyl orthosilicate (TEOS), γ-aminoproplytriethyoxy siliane(APTES), and triethyltrtramine (TETA) at 25 °C via sol-gel method on one-step. The effects of content of TEOS and coupling reagents on the mechanical and thermal properties of SiO₂/EP composites were studied. Microcosmic morphology and properties of the hybrid materials were characterized by FT-IR, TEM, FESEM, and DSC. Results revealed that SiO₂/EP composites achieve the optimal mechanical and thermal properties when the composites prepared with mass ratio of TEOS/APTES/epoxy for 3/2/100 without acetone. Compared with pristine epoxy, the tensile strength, elongation at break, impact strength and bend strength increased 67.6 %, 190 %, 82.1 % and 15.7 %, respectively. The further study was to investigate the content of TEOS and APTES effecting on mechanical properties and water sorption of fiber reinforced composites, which used the above compound as matrix resin.     

Cure retardation of peroxide‐cured silica filled natural rubber influenced by organosilane

The influence of silane coupling agent on properties of silica‐filled compounds under peroxide curing was investigated. bis (triethoxysilylpropyl) tetrasulfide (TESPT) was selected in this study and its content was varied from 0 to 12% w/w of silica. It is found that with increasing TESPT content, bound rubber content, tensile strength, elongation at break and tear strength are enhanced. By contrast, magnitude of Payne's effect, modulus at 100% elongation (M₁₀₀) and heat build‐up are decreased. The changes of such properties are attributed to the reduction of crosslink density in conjunction with the improvements of both rubber–filler interaction and degree of filler dispersion with increasing TESPT content in the peroxide curing system. POLYM. ENG. SCI., 59:42–48, 2019. © 2018 Society of Plastics Engineers     

Study of surface‐functionalized nano‐SiO2/polybenzoxazine composites

A series of the surface‐functionalized nano‐SiO₂/polybenzoxazine (PBOZ) composites was produced, and an attempt was made to improve the toughness of PBOZ material, without sacrificing other mechanical and thermal properties. A benzoxazine functional silane coupling agent was synthesized to modify the surface of nano‐SiO₂ particles, which were then mixed with benzoxazine monomers to produce the nano‐SiO₂‐PBOZ nanocomposites. The notched impact strength and the bending strength of the nano‐SiO₂‐PBOZ nanocomposites increase 40% and 50%, respectively, only with the addition of 3 wt % nano‐SiO₂. At the same load of nano‐SiO₂, the nano‐SiO₂‐PBOZ nanocomposites exhibit the highest storage modulus and glass‐transition temperature by dynamic viscoelastic analysis. Moreover, the thermal stability of the SiO₂/PBOZ nanocomposites was enhanced, as explored by the thermogravimetric analysis. The 5% weight loss temperatures increased with the nano‐SiO₂ content and were from 368°C (of the neat PBOZ) to 379°C or 405°C (of the neat PBOZ) to 426°C in air or nitrogen with additional 3 wt % nano‐SiO₂. The weight residue of the same nanocomposite was as high as 50% in nitrogen at 800°C. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Synthesis and properties of non-isocyanate aliphatic thermoplastic polyurethane elastomers with polycaprolactone soft segments

This study describes a non-isocyanate route for synthesis of aliphatic thermoplastic polyurethane elastomers (TPUEs) with excellent mechanical properties. Melt transurethane co-polycondensation of bis(hydroxyethyl) hexanediurethane with different polycaprolactone-diols was conducted at 170 °C under a reduced pressure of 3 mmHg to prepare a series of TPUEs. The TPUEs were characterized by gel permeation chromatography, FT-IR, ¹H–NMR, wide angle X-ray scattering, DSC, TGA, dynamic mechanical analysis, atomic force microscopy, SEM, and tensile analyses. The TPUEs exhibited M _n above 18,100 g/mol, T _g of ?35 to ?11 °C, T _m of up to 107 °C, initial decomposition temperature over 269 °C, tensile strength up to 32 MPa with a strain at break of 1119%, and resilience of 65% to 83%. TPUEs with good tensile strength and resilience were successfully prepared through a non-isocyanate route.     

Preparation and properties of carbon black filled EPDM/POE thermaplastic vulcanizates

TPVs filled with different amounts (0–50 phr) of carbon black were prepared via melt mixing by dynamic vulcanization in Haake plasticorder at 150°C and 40rpm and then the properties of them were studied. Torque-time curves showed that the curing degree reached a biggest value at 10 phr and then decreased with the increase of filling content while the curing rate was always rising. Mechanical properties such as tensile strength, tear strength, modulus as well as hardness increased with the increment of carbon black content while the tension set at break was reduced dramatically. Two phase morphology was observed by SEM photographs and the effect of carbon black on curing extent was testified. To illuminate the effect of carbon black, curometer curves and carbon black dispersion pictures were also analyzed. Rubber processing analyzer (RPA) experiments proved that there was a progressive nonlinear behavior, which was more and more clearly expressed with the increment of carbon black content and could be explained via the Payne effect. But the TPVs containing highest carbon black exhibited the fastest drop of G′ with increasing strain amplitude as obtained from the value of G₀′ − G_∞′. The order of tanδ at different carbon black content was tanδ (10 phr) < tanδ (0 phr) < tanδ (30 phr) < tanδ (50 phr) at lower strain amplitude. © 2012 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Adhesion properties and fracture mechanism of plasma sprayed NiCrAl/Al2O3–13wt.%TiO2 coatings by post annealing

Plasma-sprayed NiCrAl/Al₂O₃–13wt.%TiO₂ coatings (AT13) deposited on mild steel substrate were annealed with varying temperatures in air. The adhesion of the coating was evaluated by tensile adhesive strength test. The microstructure and the fracture mechanism were studied using optical microscopy, X-ray diffraction, and scanning electron spectroscopy/energy dispersive spectroscopy. It was found that the tensile bond strength of the coatings increased with increasing of annealing temperature at first and then decreased with increasing of annealing temperature further. The as-sprayed coating fractured at the interfaces of substrate/bond layer and bond layer/ceramic coating with a brittle–ductile mixed fracture. The measured strength expressed the adhesive strength and internal adhesive strength of the coating. The failure of the coating annealed at 300, 400, and 500 °C took place at the interface of substrate/bond layer and had a mixed fracture surface of transgranular cleavage fracture and localized ductile fracture. The strength obtained is the adhesive strength between the coating and the steel substrate. The coating annealed at 400 °C had a maximum strength of 42.9 MPa. When the temperature is above 600 °C, the bonding strength would be damaged. Therefore, there is a proper annealing temperature which can significantly improve the bond strength of the coating.     

Low-temperature thermally modified fir-derived biomorphic C–SiC composites prepared by sol-gel infiltration

In order to solve the problems (i.e. low infiltration efficiency, cracks, interface separation and poor mechanical properties) in the process of wood-derived C–SiC composites, the thermal modification of fir at low temperatures (300 °C ～ 350 °C) combined with sol-gel infiltration was used to successfully produce biomorphic ceramics. The prepared materials were comprehensively characterized and exhibited improved interfacial bonding between C and SiC and mechanical properties. The weight gain per unit volume (0.123 g/cm³) of SiO₂ gel in the fir thermally modified at 300 °C is 167.4%, higher than that (0.046 g/cm³) of the unmodified fir. A well-bonded interface was formed between the SiO₂ gel and the pore wall of the fir thermally modified at 300 °C. With the increase of modification temperature from 300 °C to 350 °C, the distance between SiO₂ gel and the pore wall increases, and a gap (1–3 μm) is observed between SiO₂ gel and the pore wall of the fir carbonized at 600 °C. The C–SiC composites sintered at 1400 °C exhibited the highest compressive strength and bending strength of 40.8 ± 5.8 MPa and 11.7 ± 2.1 MPa, respectively, owing to the well-bonded interface between C of fir thermally modified at 300 °C and SiC. However, the composites sintered at 1600 °C for 120 min exhibited the lowest compressive strength and bending strength of 28.1 ± 13.4 MPa and 5.7 ± 1.6 MPa, respectively, which are 31.1% and 51.3% lower than those sintered at 1400 °C for 120 min, respectively. This might result from the porous structure formed by the excessive consumption of fir-derived carbon during the reaction between C and SiO₂ at 1600 °C for 120 min. Therefore, thermal modification in the preparation of biomorphic C–SiC composites can promote slurry infiltration and the formation of a well-bonded interface between C and SiC, thus improving the mechanical properties of the composites.     

Effect of CaO/SiO2 ratio on phase transformation and properties of anorthite-based ceramics from coal fly ash and steel slag

Anorthite-based ceramics were produced entirely from coal fly ash and steel slag. The effect of the CaO/SiO₂ ratio (0.12–0.8) on the phase transitions was examined by adding steel slag to coal fly ash in the range of 10–50 wt%, and a temperature range of 900–1200 °C. The influence of CaO/SiO₂ and sintering temperatures on the technological properties were assessed by response surface methodology (RSM) and correlated with the phase changes. The results revealed that anorthite was the main phase for the CaO/SiO₂ ratio ranging from 0.12 to 0.56, while at 1200 °C, a ratio of 0.8 involved a high content of gehlenite. RSM showed that the CaO/SiO₂ ratio was the main influencing factor on the density, while the variation of apparent porosity and compressive strength were more affected by sintering temperature. The crystallisation of the anorthite phase significantly enhanced the properties of the obtained ceramics, whereas the appearance of gehlenite reduced the mechanical strength. The optimum conditions to fabricate anorthite-based ceramics with suitable properties were found to be a CaO/SiO₂ ratio of 0.46 and a temperature of 1188 °C. The optimised anorthite-based ceramic exhibited a low thermal conductivity (0.39 W/m.K) and a dielectric constant of 6.03 at 1 MHz, along with a compressive strength of 41 MPa, which makes this sample a potential candidate for insulator applications.     

Effect of chemical interaction on morphology and mechanical properties of CPI‐OH/SiO2 hybrid films with coupling agent

A novel hybrid film composed of copolyimide with hydroxyl group, silica and γ‐glycidyloxypropyltrimethoxysilane (CPI‐OH/SiO₂/GOTMS) was prepared by the sol–gel process based on hydrolyzed tetraethoxysilane (TEOS) under acidic condition. GOTMS, as the coupling agent, and hydroxyl group in PI chain were used to improve the compatibility between the PI and SiO₂. The components, morphologies, and mechanical properties of the hybrids were investigated by FTIR, UV–vis, SEM, stress–strain tests, and DMA. The results showed that SiO₂ particle size significantly decreased, fractured cross sections of hybrid were rougher, and the surfaces of spherical SiO₂ particles were more widely covered by PI component. The tensile mechanical properties of hybrids increased when adding GOTMS. The critical points of maximum tensile strength and elongation at break move from 11 to 16 wt % SiO₂ content. DMA results showed that the storage moduli of hybrids with GOTMS, when above 260°C, were obviously higher than those without GOTMS; the tan δ transition temperature of hybrid films went up from 317 to 337°C. It suggests that chemical interaction between CPI‐OH and SiO₂ is formed and the PI molecular mobility is restricted by the chemical interaction. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci 104: 3530–3538, 2007