Flexible cellulose composite film incorporated by carbon nitride@graphene oxide prepared by a “compressed-aerogel” approach for efficient thermal management

Heat dissipation films originating from polymer composite with improved thermal conductivity are becoming potential candidates for effective thermal management of next-generation electronic products, profiting from their soft nature and good electrical insulation. In this work, a novel hybrid filler composed of carbon nitride (C₃N₄) and graphene oxide (GO) is synthesized and further introduced into the cellulose matrix. The electrical insulation of the composite is maintained, attributed to the low electrical conductivity of C₃N₄. Meanwhile, the bridged chemical bond between C₃N₄ and GO reduces the interfacial thermal resistance and promotes heat transfer. By hot-pressing the aerogel intermediate, the directional arrangement of fillers is achieved, leading to favorable flexibility and mechanical behavior, and superior in-plane thermal conductivity (5.74 W/mK) of the composite. Thermal characterizations reveal that lower thermal contact resistance (TCR), improved thermal stability, and the relatively lower coefficient of thermal expansion (CTE) together facilitate its practical application in thermal management. The practical performance test is also performed which fully demonstrates its favorable temperature regulation ability, reflected by a 2.7 °C temperature decrement observed in the cell phone battery heat dissipation test.     

High thermal conductive epoxy molding compound with thermal conductive pathway

The epoxy molding compound (EMC) with thermal conductive pathways was developed by structure designing. Three kinds of EMCs with different thermal conductivities were used in this investigation, specifically epoxy filled with Si₃N₄, filled with hybrid Si₃N₄/SiO₂, and filled with SiO₂. Improved thermal conductivity was achieved by constructing thermal conductive pathways using high thermal conductivity EMC (Si₃N₄) in low thermal conductivity EMC (SiO₂). The morphology and microstructure of the top of EMC indicate that continuous network is formed by the filler which anticipates heat conductivity. The highest thermal conductivity of the EMC was 2.5 W/m K, reached when the volume fraction of EMC (Si₃N₄) is 80% (to compare with hybrid Si₃N₄/SiO₂ filled‐EMC, the content of total fillers in the EMC was kept at 60 vol %). For a given volume fraction of EMC (Si₃N₄) in the EMC system, thermal conductivity values increase according to the order EMC (Si₃N₄) particles filled‐EMC, hybrid Si₃N₄/SiO₂ filled‐EMC, and EMC(SiO₂) particles filled‐EMC. The coefficient of thermal expansion (CTE) decreases with increasing Si₃N₄ content in the whole filler. The values of CTE ranged between 23 × 10^?6 and 30 × 10^?6 K^?1. The investigated EMC samples have a flexural strength of about 36–39 MPa. The dielectric constant increases with Si₃N₄ content but generally remains at a low level (<6, at 1 MHz). The average electrical volume resistivity of the EMC samples are higher than 1.4 × 10¹⁰ Ω m, the average electrical surface resistivity of the EMC samples are higher than 6.7 × 10¹⁴ Ω. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Preparation of functional reduced graphene oxide and its influence on the properties of polyimide composites

Homogeneous dispersion and strong filler–matrix interfacial interactions were vital factors for graphene for enhancing the properties of polymer composites. To improve the dispersion of graphene in the polymer matrix and enhance the interfacial interactions, graphene oxide (GO), as an important precursor of graphene, was functionalized with amine‐terminated poly(ethylene glycol) (PEG–NH₂) to prepare GO–poly(ethylene glycol) (PEG). Then, GO–PEG was further reduced to prepare modified reduced graphene oxide (rGO)–PEG with N₂H₄·H₂O. The success of the modification was confirmed by Fourier transform infrared spectroscopy, thermogravimetric analysis, and Raman spectroscopy. Different loadings of rGO–PEG were introduced into polyimide (PI) to produce composites via in situ polymerization and a thermal reduction process. The modification of PEG–NH₂ on the surface of rGO inhibited its reaggregation and improved the filler–matrix interfacial interactions. The properties of the composites were enhanced by the incorporation of rGO–PEG. With the addition of 1.0 wt % rGO–PEG, the tensile strength of PI increased by 81.5%, and the electrical conductivity increased by eight orders of magnitude. This significant improvement was attributed to the homogeneous dispersion of rGO–PEG and its strong filler–matrix interfacial interactions. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45119.     

Thermal,electrical, and mechanical properties of Si3N4 filled LLDPE composite

Silicon nitride (Si₃N₄) filled linear low-density polyethylene (LLDPE) composite was prepared. The effects of Si₃N₄ filler content, dispersion, and LLDPE particle size on the thermal conductivity, and Si₃N₄ filled content on the mechanical and electrical properties of Si₃N₄ reinforced LLDPE composites prepared using powder mixing were investigated. The results indicate that there existed a unique dispersion state of Si₃N₄ particles in LLDPE, shell-kernel structure, in which Si₃N₄ particles surrounded LLDPE matrix particles. With increasing filler content and LLDPE particles size, thermal conductivity increased, and reached 1.42 W/m K at 30 vol% of filler, seven times as that of unfilled LLDPE. Furthermore, the examinations of Agari model demonstrate that larger size LLDPE particles form thermal conductive networks easily compared with smaller ones. The values predicted by theoretical model underestimate the thermal conductivity of Si₃N₄/LLDPE composites. In addition, the composites still possessed rather higher electrical resistivity and dielectric properties, but the mechanical properties decreased. POLYM. COMPOS., 2009. © 2008 Society of Plastics Engineers     

Experimental and theoretical studies on the adjustable thermal properties of epoxy composites with silver‐plated short fiberglass

This article investigates the evolution of the thermal conductivity and the coefficient of thermal expansion (CTE) of epoxy composites filled with different silver‐plated short glass fibers (Ag@GFs) treated by electroless plating. After electroless plating, the results of X‐ray diffraction and scanning electron microscopy showed that glass fibers were coated with pure silver shells whose thickness was controlled via the repetition of electroless plating cycle, and calculated by weighting method. The optical photographs showed that Ag@GFs are randomly oriented and uniformly dispersed in the composites. HotDisk thermal constant analyzer and dilatometer were used to further characterize the thermal conductivity and the CTE of the composites, respectively. The results revealed that the thermal conductivity of Ag@GF/epoxy composites increased with the increase of Ag@GF content, and was adjusted by changing the thickness of silver shell. But the CTE of the composites drops sharply as the Ag@GF content increases compared with neat epoxy. Based on Agari model with fitted factors of C_p and C_f, the calculated thermal conductivity values of Ag@GF/epoxy composites agreed well with the experimental results, and C_p kept almost unchanged, but C_f varied with the change of the thickness of silver shell, despite increasing filler content. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45555.     

Enhanced tribological performance of hybrid polytetrafluoroethylene/Kevlar fabric composite filled with milled pitch‐based carbon fibers

As self‐lubricating bearing liner materials, tribological properties of milled pitch‐based carbon fibers (CFs) modified polytetrafluoroethylene (PTFE)/Kevlar fabric composites were investigated, and the microscopic morphology of worn surface was studied. The results show that the appropriate incorporation of CFs can obviously reduce the wear rate of the fabric composite with almost unchanging friction coefficient. The wear rates of 5 wt % CF‐filled PTFE/Kevlar fabric composites are decreased by 30% and 48% for two kinds of composites made with fibers from different producers compared with unfilled fabric composites. Scanning electron microscopy observations show that the appropriate incorporation of CFs obviously improves the interfacial bonding and reduces pull‐out and fracture of Kevlar fiber. Meanwhile, the introduction of CFs at proper fraction is helpful to form smooth and continuous transfer film on the surface of metal counterpart. The improving mechanism of the CF is attributed to increasing mechanical strength, thermal conductivity and self‐lubricating effects. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 46269.     

An investigation on the graphitic carbon nitride reinforced polyimide composite and evaluation of its tribological properties

This article presented a novel application for the graphitic carbon nitride (g‐C₃N₄), which was used as nanofillers to improve the tribological properties of polyimide (PI). The composite based on PI and g‐C₃N₄ was prepared by mechanical mixing process and hot compression molding process. The characterizations of g‐C₃N₄ and PI/g‐C₃N₄ composites were investigated by Fourier transform infrared spectroscopy, X‐ray diffraction, thermogravimetric analysis, and scanning electron microscopy. Friction and wear tests were carried out using UMT‐2 reciprocating tribo‐tester against stainless steel ball under dry friction. The results showed that the amount of g‐C₃N₄ was decisive to the tribological properties of PI/g‐C₃N₄ composites. The optimal tribological properties occurred when the amount of g‐C₃N₄ was 10 wt %, which showed the smallest friction coefficient and the lowest wear rate. Furthermore, this work provided an example of application for the g‐C₃N₄ as the excellent nanofiller in polymer matrix composites. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45403.     

Synthesis of conducting graphene/Si3N4 composites by spark plasma sintering

Graphene/silicon nitride (Si₃N₄) composites with high fraction of few layered graphene are synthesized by an in situ reduction of graphene oxide (GO) during spark plasma sintering (SPS) of the GO/Si₃N₄ composites. The adequate intermixing of the GO layers and the ceramic powders is achieved in alcohol under sonication followed by blade mixing. The reduction of GO occurs together with the composite densification in SPS, thus avoiding the implementation of additional reduction steps. The materials are studied by X-ray photoelectron and micro-Raman spectroscopy, revealing a high level of recovery of graphene-like domains. The SPS graphene/Si₃N₄ composites exhibit relatively large electrical conductivity values caused by the presence of reduced graphene oxide (∼1 S cm⁻¹ for ∼4 vol.%, and ∼7 S cm⁻¹ for 7 vol.% of reduced-GO). This single-step process also prevents the formation of highly curved graphene sheets during the thermal treatment as the sheets are homogeneously embedded in the ceramic matrix. The uniform distribution of the reduced GO sheets in the composites also produces a noticeable grain refinement of the silicon nitride matrix.     

Effect of oxygen functional groups of reduced graphene oxide on the mechanical and thermal properties of polypropylene nanocomposites

Reduced graphene oxide (rGO) with various surface structures was prepared by reducing graphene oxide (GO) with hydrazine hydrate (N₂H₄), sodium borohydride (NaBH₄) and l ‐ascorbic acid, respectively. The resulting rGO were used to fabricate rGO/polypropylene (PP) nanocomposites by a melt‐blending method. The surface structure of rGO as well as multifunctional properties of rGO/PP nanocomposites were thoroughly investigated. It was shown that rGO with highest C/O ratio could be obtained by reducing GO with N₂H₄. The crystallization behaviors, tensile strength, thermal conductivity and thermal stability of rGO/PP nanocomposites were significantly improved with the increase of C/O ratio of rGO. For example, with only 1 phr (parts per hundred PP) rGO reduced by N₂H₄, the degree of crystallinity, tensile strength, maximum heat decomposition temperature and thermal conductivity of PP nanocomposite were increased by 6.2%, 20.5%, 48.0 °C and 54.5%, respectively, compared with those of pure PP. Moreover, the thermal degradation kinetics indicated that the decomposition activation energy of rGO/PP nanocomposites could be enhanced by adding rGO with higher C/O ratio. © 2018 Society of Chemical Industry     

Preparation of cellulose–graphene oxide aerogels with N‐methyl morpholine‐N‐oxide as a solvent

Cellulose–graphene oxide (GO) aerogel composites were successfully prepared from cellulose and GO dispersed in N‐methyl morpholine‐N‐oxide monohydrate, a nontoxic and environmentally friendly solvent, after a freeze‐drying process. Because of the strong interactions between the numerous oxygen‐containing groups located on the surface of GO and the functional groups of the cellulose molecules, the GO monolayers were well dispersed in the three‐dimensional porous structure of the cellulose aerogels. With the addition of 10 wt % GO, the swelling ratios and water contents of the composite cellulose–GO aerogels increased from 468 to 706% and from 82.4% to 87.6%, respectively. The corresponding maximum decomposition temperatures also increased from 335 to 353 °C with increasing GO content from 0 to 10%; this indicated that the thermal stability of the cellulose–GO aerogels was enhanced. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 46152.     

Thermal and mechanical properties of liquid silicone rubber composites filled with functionalized graphene oxide

To improve the thermal and mechanical properties of liquid silicone rubber (LSR) for application, the graphene oxide (GO) was proposed to reinforce the LSR. The GO was functionalized with triethoxyvinylsilane (TEVS) by dehydration reaction to improve the dispersion and compatibility in the matrix. The structure of the functionalized graphene oxide (TEVS‐GO) was evaluated by Thermogravimetric analysis (TGA), Fourier transform infrared (FTIR) spectra, X‐ray diffraction (XRD), and energy dispersive X‐ray spectroscopy (EDX). It was found that the TEVS was successfully grafted on the surface of GO. The TEVS‐GO/LSR composites were prepared via in situ polymerization. The structure of the composites was verified by FTIR, XRD, and scanning electron microscopy (SEM). The thermal properties of the composites were characterized by TGA and thermal conductivity. The results showed that the 10% weight loss temperature (T₁₀) increased 16.0°C with only 0.3 wt % addition of TEVS‐GO and the thermal conductivity possessed a two‐fold increase, compared to the pure LSR. Furthermore, the mechanical properties were studied and results revealed that the TEVS‐GO/LSR composites with 0.3 wt % TEVS‐GO displayed a 2.3‐fold increase in tensile strength, a 2.79‐fold enhancement in tear strength, and a 1.97‐fold reinforcement in shear strength compared with the neat LSR. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42582.     

Noncovalent functionalization of carbon nanotubes using branched random copolymer for improvement of thermal conductivity and mechanical properties of epoxy thermosets

A branched random copolymer, poly[(hydroxyethyl acrylate)‐r‐(N‐vinylcarbazole)] (BPHNV), was synthesized through a facile one‐pot free radical polymerization with hydroxyethyl acrylate and N‐vinylcarbazole monomers, using 4‐vinylmethylmercaptan as the chain transfer agent. BPHNV was employed to noncovalently modify multiwall carbon nanotubes (MWCNTs) by π–π interaction. The as‐modified MWCNTs were then incorporated into epoxy resin to improve the thermal conductivity and mechanical properties of epoxy thermosets. The results suggest that, due to both the conjugation structure and the epoxy‐philic component, BPHNV could form a polymer layer on the wall of MWCNTs and inhibit entanglement, helping the uniform dispersion of MWCNTs in epoxy matrix. Owing to the unprecedented thermal conductivity of MWCNTs and the enhancement in the interfacial interaction between fillers and matrix, the thermal conductivity of epoxy/MWCNTs/BPHNV composites increases by 78% at extremely low filler loadings, while the electrical resistivity is still maintained on account of the insulating polymer layer. Meanwhile, the mechanical properties and glass transition temperature (T_g) of the thermosets are elevated effectively, with no significant decrease occurring to the modulus. The addition of as little as 0.1 wt% of MWCNTs decorated with 1.0 wt% of BPHNV to an epoxy matrix affords a great increase of 130% in impact strength for the epoxy thermosets, as well as an increase of over 13 °C in T_g. © 2018 Society of Chemical Industry     

Preparation and properties of dopamine reduced graphene oxide and its composites of epoxy

To improve the thermal and mechanical properties and further to expand its applications of epoxy in electronic packaging, reduced graphene oxide/epoxy composites have been successfully prepared, in which dopamine (DA) was used as reducing agent and modifier for graphene oxide (GO) to avoid the environmentally harmful reducing agents and address the problem of aggregation of graphene in composites. Further studies revealed that DA could effectively eliminate the labile oxygen functionality of GO and generate polydopamine functionalized graphene oxide (PDA‐GO) because DA would be oxidated and undergo the rearrangement and intermolecular cross‐linking reaction to produce polydopamine (PDA), which would improve the interfacial adhesion between GO and epoxy, and further be beneficial for the homogenous dispersion of GO in epoxy matrix. The effect of PDA‐GO on the thermal and mechanical properties of PDA‐GO/epoxy composites was also investigated, and the incorporation of PDA‐GO could increase the thermal conductivity, storage modulus, glass transition (T_g), and dielectric constant of epoxy. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 39754.     

Simultaneously enhanced mechanical properties and thermal properties of ultrahigh‐molecular‐weight polyethylene with polydopamine‐coated α‐alumina platelets

Polydopamine (PDA) was employed to modify micrometric Al₂O₃ platelets to improve the interfacial compatibility between α‐Al₂O₃ powder and ultrahigh‐molecular‐weight polyethylene (UHMWPE). The structure of PDA‐coated Al₂O₃ and UHMWPE composites was investigated via Fourier transform infrared spectroscopy, scanning electron microscopy and X‐ray photoelectron spectroscopy. The thermal stability and mechanical performance of the samples were also evaluated. It is clear that UHMWPE/PDA‐Al₂O₃ composites exhibit better mechanical properties, higher thermal stability and higher thermal conductivity than UHMWPE/Al₂O₃ composites, owing to the good dispersion of Al₂O₃ powder in the UHMWPE matrix and the strong interfacial force between the macromolecules and the inorganic filler caused by the presence of PDA. The tensile strength and the tensile elongation at break of UHMWPE/PDA‐Al₂O₃ composite with 1 wt% PDA‐Al₂O₃ are 62.508 MPa and 462%, which are 1.96 and 1.98 times higher than those of pure UHMWPE, respectively. The thermal conductivity of UHMWPE/PDA‐Al₂O₃ composite increases from 0.38 to 0.52 W m^?1 K^?1 with an increase in the dosage of PDA‐Al₂O₃ to 20 wt%. The results show that the prepared PDA‐coated Al₂O₃ powder can simultaneously enhance the mechanical properties and thermal conductivity of UHMWPE. © 2018 Society of Chemical Industry     

Synthesis and properties of AlN/MAS/Si3N4 ternary glass-ceramic composites with in-situ grown rod-like β-Si3N4 crystals

The AlN/MAS/Si₃N₄ ternary composites with in-situ grown rod-like β-Si₃N₄ were obtained by a two-step sintering process. The microstructure analysis, compositional investigation as well as properties characterization have been systematically performed. The AlN/MAS/Si₃N₄ ternary composites can be densified at 1650 °C in nitrogen atmosphere. The in-situ grown rod-like β-Si₃N₄ grains are beneficial to the improvement of thermal, mechanical, and dielectric properties. The thermal conductivity of the composites was increased from 14.85 to 28.45 W/(m K) by incorporating 25 wt% α-Si₃N₄. The microstructural characterization shows that the in-situ growth of rod-like β-Si₃N₄ crystals leads to high thermal conductivity. The AlN/MAS/Si₃N₄ ternary composite with the highest thermal conductivity shows a low relative dielectric constant of 6.2, a low dielectric loss of 0.0017, a high bending strength of 325 MPa, a high fracture toughness of 4.1 MPa m^1/2, and a low thermal expansion coefficient (α_{25–300 °C}) of 5.11 × 10^?6/K. This ternary composite with excellent comprehensive performance is expected to be used in high-performance electronic packaging materials.     

Thermal properties of polytetrafluoroethylene/Sr2Ce2Ti5O16 polymer/ceramic composites

Polytetrafluoroethylene (PTFE) composites filled with Sr₂Ce₂Ti₅O₁₆ ceramic were prepared by a powder processing technique. The structures and microstructures of the composites were investigated by X‐ray diffraction and scanning electron microscopy techniques. Differential scanning calorimetry showed that the ceramic filler had no effect on the melting point of the PTFE. The effect of the Sr₂Ce₂Ti₅O₁₆ ceramic content [0–0.6 volume fraction (vf)] on the thermal conductivity, coefficient of thermal expansion (CTE), specific heat capacity, and thermal diffusivity were investigated. As the vf of the Sr₂Ce₂Ti₅O₁₆ ceramic increased, the thermal conductivity of the specimen increased, and the CTE decreased. The thermal conductivity and thermal expansion of the PTFE/Sr₂Ce₂Ti₅O₁₆ composites were improved to 1.7 W m^?1 °C^?1 and 34 ppm/°C, respectively for 0.6 vf of the ceramics. The experimental thermal conductivity and CTE were compared with different theoretical models. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Mechanical and thermal properties of hierarchical composites enhanced by pristine graphene and graphene oxide nanoinclusions

Epoxy resin nanocomposites incorporated with 0.5, 1, 2, and 4 wt % pristine graphene and modified graphene oxide (GO) nanoflakes were produced and used to fabricate carbon fiber‐reinforced and glass fiber‐reinforced composite panels via vacuum‐assisted resin transfer molding process. Mechanical and thermal properties of the composite panels—called hierarchical graphene composites—were determined according to ASTM standards. It was observed that the studied properties were improved consistently by increasing the amount of nanoinclusions. Particularly, in the presence of 4 wt % GO in the resin, tensile modulus, compressive strength, and flexural modulus of carbon fiber (glass fiber) composites were improved 15% (21%), 34% (84%), and 40% (68%), respectively. Likewise, with inclusion of 4 wt % pristine graphene in the resin, tensile modulus, compressive strength, and flexural modulus of carbon fiber (glass fiber) composites were improved 11% (7%), 30% (77%), and 34% (58%), respectively. Also, thermal conductivity of the carbon fiber (glass fiber) composites with 4% GO inclusion was improved 52% (89%). Similarly, thermal conductivity of the carbon fiber (glass fiber) composites with 4% pristine graphene inclusion was improved 45% (80%). The reported results indicate that both pristine graphene and modified GO nanoflakes are excellent options to enhance the mechanical and thermal properties of fiber‐reinforced polymeric composites and to make them viable replacement materials for metallic parts in different industries, such as wind energy, aerospace, marine, and automotive. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 40826.     

Tunable microwave absorption performance of carbon fiber-reinforced reaction bonded silicon nitride composites

The hybrid network of Si₃N₄ whiskers and conducting carbon fiber has great potential for microwave absoprtion applications. The high electrical conductivity of the carbon fiber helps to transform the microwave transparent Si₃N₄ into microwave absorbing materials. Herein, the microwave absorption performance of 5–20 vol % of carbon fiber reinforced reaction bonded Si₃N₄ (C_f-RBSN) composites have been discussed in detail. The C_f reinforcement tuned the X-band dielectric properties of the RBSN composites. The 5 vol % C_f-RBSN composite exhibit a minimum reflection loss (RL_min) of ?36.16 dB (99.998% microwave absorption) at 11.89 GHz and a high specific reflection loss of 920 dB. g^?1 for 5.9 mm thickness, while 20 vol % C_f-RBSN composites resulted in RL_min of ?22.86 dB at 11.56 GHz with a low thickness of 1.5 mm. Thus, the superior microwave absorption performance of the prepared lightweight composites results from the multiple interfacial polarization, dipole polarization, and conduction loss due to the 3D network of interconnected Si₃N₄ whiskers and C_f.     

Enhanced thermal conductivity and dimensional stability of flexible polyimide nanocomposite film by addition of functionalized graphene oxide

Polyimide (PI) nanocomposites with both enhanced thermal conductivity and dimensional stability were achieved by incorporating glycidyl methacrylate‐grafted graphene oxide (g‐GO) in the PI matrix. The PI/g‐GO nanocomposites exhibited linear enhancement in thermal conductivity when the amount of incorporated g‐GO was less than 10 wt%. With the addition of 10 wt% of g‐GO to PI (PI/g‐GO‐10), the thermal conductivity increased to 0.81 W m^?1 K^?1 compared to 0.13 W m^?1 K^?1 for pure PI. Moreover, the PI/g‐GO‐10 composite exhibited a low coefficient of thermal expansion (CTE) of 29 ppm °C^?1. The values of CTE and thermal conductivity continuously decreased and increased, respectively, as the g‐GO content increased to 20 wt%. Combined with excellent thermal stability and high mechanical strength, the highly thermally conducting PI/g‐GO‐10 nanocomposite is a potential substrate material for modern flexible printed circuits requiring efficient heat transfer capability.     

Mechanical and thermal properties of biphenyldiol formaldehyde resin/gallic acid epoxy composites enhanced by graphene oxide

In this study, the gallic acid‐based epoxy resin (GA‐ER) and alkali‐catalysed biphenyl‐4,4′‐diol formaldehyde resin (BPFR) are synthesized. Glass fibre‐reinforced GA‐ER/BPFR composites are prepared. Graphene oxide (GO) is used to improve the mechanical and thermal properties of GA‐ER/BPFR composites. Dynamic mechanical properties and thermal, mechanical, and electrical properties of the composites with different GO content are characterized. The results demonstrate that GO can enhance the mechanical and thermal properties of the composites. The glass transition temperature, T_g, of the BPFR/GA‐ER/GO composites is 20.7°C higher than the pure resin system, and the 5% weight loss temperature, T_d5, is enhanced approximately 56.6°C. When the BPFR: GA‐ER mass ratio is at 4 : 6 and GO content is 1.0–1.2 wt %, the tensile and impact strengths of composites are 60.97 MPa and 32.08 kJ/m² higher than the pure resin composites, respectively. BPFR/GA‐ER composites have better mechanical properties, and can replace common BPA epoxy resins in the fabrication of composites. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42637.