Graphene‐based composite with microwave absorption property prepared by in situ reduction

Binary composite of graphene/poly(ethylene oxide) (PEO) with microwave absorption property is prepared by in situ reduction process. Graphite oxide (GO) is prepared from flake graphite by modified Hummers' method and further dispersed in distilled water to get GO solution. Then, PEO powder is slowly added into GO solution to get GO/PEO solution, and graphene/PEO composites is prepared via a facile and quick reduction process in GO/PEO solution. PEO and graphene/PEO composites are characterized by scanning electron microscopy, atomic force microscopy, thermo gravimetric analysis, and vector network analyzer. The results show that graphene is uniformly dispersed in PEO matrix because GO and PEO can be uniformly dispersed at molecular level due to their water‐solubility and the agglomeration of graphene can be prevented by PEO macromolecular chains during in situ reduction process. Graphene/PEO composite has better thermal stability than PEO, which can be explained by the graphene restoration of sp² bonded carbon structure. Meanwhile, graphene/PEO composite shows excellent microwave absorption property at low grapheme content. The minimum reflection loss of graphene/PEO composite is up to −20.0 dB when the content of graphene is only 1 wt%. POLYM. COMPOS., 35:461–467, 2014. © 2013 Society of Plastics Engineers     

Electrical conductivity studies on water‐soluble polypyrrole–graphene oxide composites

Polypyrrole (PPy)–graphene oxide (GO) composites are synthesized via a soft‐chemical in situ method at different GO concentrations (10, 20, 30, 40, and 50 wt%) and with ammonium persulfate (APS) as the oxidant. The synthesized composites were characterized using Fourier transform infrared (FTIR) and ultraviolet‐visible light (UV–vis) spectroscopic studies, and their surface properties were analyzed using scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Characterization and surface morphology results indicate that PPy is adsorbed onto the graphene surfaces and/or fills the GO sheets. The temperature‐dependent DC conductivity of the polymer composite films in the 300–500 K range indicates a semiconducting behavior with increasing GO concentration in the PPy polymer. Based on morphological and conductivity studies, the large surface area and high aspect ratio of the in situ‐generated GO may have played an important role in the noticeable improvement in the electrical conductivity of the prepared composites. POLYM. COMPOS., 2011. © 2011 Society of Plastics Engineers     

Reinforced polystyrene via solvent‐exfoliated graphene

Solvent‐exfoliated graphene (SEG)‐reinforced polystyrene (PS) composites were prepared using a straightforward solution‐casting method. SEG sheets, obtained by sonication‐assisted solvent direct exfoliation from natural graphite, were well dispersed in the PS matrix as evidenced from scanning electron microscopy and transmission electron microscopy observations. Addition of 0.5 wt% SEG resulted in a 6% increase in tensile strength and a 77% improvement in Young's modulus over pure PS due to the effective load transfer between SEG and PS matrix. The Young's moduli of the PS/SEG composites were obtained from both tensile experiments and calculations using the well‐established Halpin–Tsai model. Results from dynamic mechanical analysis indicated that the storage modulus of the PS/SEG composites was significantly improved relative to neat PS. The glass transition temperatures of the composites were found to increase substantially upon addition of SEG, consistent with differential scanning calorimetry analysis. © 2017 Society of Chemical Industry     

SiCNO–GO composites with the negative temperature coefficient of resistance for high‐temperature sensor applications

We report the synthesis of silicon oxycarbonitride ceramic‐graphene oxide (SiCNO–GO) composites by using polyvinylsilazne (PVSZ) and GO as precursors through cross‐linking processes, in which GO organizes into microspheres in the SiCNO matrix. The formation of GO microspheres significantly enhances the electrical conductivity of SiCNO. The electrical resistivity of SiCNO–GO composites shows a negative temperature coefficient in the range from 25°C to 600°C. We demonstrate the application of SiCNO–GO composites as the functional component of high‐temperature sensors.     

In situ thermal reduction of graphene oxide in a styrene–ethylene/butylene–styrene triblock copolymer via melt blending

We report an in situ thermal reduction of graphene oxide (GO) in a styrene–ethylene/butylene–styrene (SEBS) triblock copolymer matrix during a melt‐blending process. A relatively high degree of reduction was achieved by melt‐blending premixed GO/SEBS nanocomposites in a Haake mixer for 25 min at 225 °C. Infrared spectral results revealed the successful thermal reduction of, and the strong adsorption of SEBS on, the graphene sheets. The glass transition temperature of polystyrene (PS) segments in SEBS was enhanced by the incorporation of thermally reduced graphene oxide (TRGO). The resultant TRGO/SEBS nanocomposites were used as a masterbatch to improve the mechanical properties of PS. Both the elongation at break and the flexural strength of PS/SEBS blends were enhanced with the addition of the TRGO. Our demonstration of the in situ thermal reduction of GO via melt blending is a simple, efficient strategy for preparing nanocomposites with well‐dispersed TRGO in the polymer matrix, which could be an important route for large‐scale fabrication of high‐performance graphene/polymer nanocomposites. © 2013 Society of Chemical Industry     

Processing–Nanostructure–Property Relationships of All‐Polyethylene Composites Reinforced by Flow‐Induced Oriented Crystallization of UHMWPE

All‐polyethylene composites exhibiting substantially improved toughness/stiffness balance are readily produced during conventional injection molding of high density polyethylene (HDPE) in the presence of bimodal polyethylene reactor blends (RB40) containing 40 wt% ultrahigh molar mass polyethylene (UHMWPE) dispersed in HDPE wax. Scanning electron microscopy (SEM) and differential scanning calorimetry (DSC) analyses shows that flow‐induced crystallization affords extended‐chain UHMWPE nanofibers forming shish which nucleates HDPE crystallization producing shish‐kebab structures as reinforcing phases. This is unparalleled by melt compounding micron‐sized UHMWPE. Injection molding of HDPE with 30 wt% RB40 at 165 °C affords thermoplastic all‐PE composites (12 wt% UHMWPE), improved Young's modulus of 3400 MPa, tensile strength of 140 MPa, and impact resistance of 22.0 kJ/m². According to fracture surface analysis, the formation of skin‐intermediate‐core structures accounts for significantly improved impact resistance. At constant RB40 content both morphology and mechanical properties strongly depend upon processing temperature. Upon increasing processing temperature from 165 °C to 250 °C the average shish‐kebab diameter increases from the nanometer to micron range, paralleled by massive loss of self‐reinforcement above 200 °C. The absence of shish‐kebab structure at 250 °C is attributed to relaxation of polymer chains and stretch‐coil transition impairing shish formation.     

Effect of Dodecyal Amine Functionalized Graphene on the Mechanical and Thermal Properties of Epoxy‐Based Composites

Simultaneous surface functionalization and reduction of graphene oxide (GO) was achieved by using dodecyl amine (DA) as surface modifying agent. The DA modified reduced GO (DA‐G) was used for subsequent preparation of DA‐G/epoxy composites by solution mixing. Fourier transform infrared spectroscopy analysis, X‐ray diffraction (XRD) and electrical conductivity measurements were conducted to establish the concurrent functionalization and reduction of GO. The effect of DA‐G on the epoxy composites at 0 to 0.75 wt% loadings was studied by investigating its static and dynamical mechanical properties. XRD study was performed to verify the dispersion of DA‐G in the epoxy polymer. Field emission scanning electron microscopy was used to investigate the fracture surface morphology of the composites and Transmission electron microscopy was employed to further confirm the dispersion of DA‐G in the matrix. It was found that the tensile strength of the composite was increased by 38.8% with the addition of 0.5 wt% of DA‐G. The good adhesion/interaction between DA‐G and epoxy resulted in the increase of storage modulus; however, glass transition temperature (T_g) value of the composites shifted to lower temperature in comparison to the neat epoxy. Thermogravimetric analysis showed small decrease in onset degradation temperature for the composites as compared to neat epoxy except for the composites containing 0.75 wt% of DA‐G. POLYM. ENG. SCI., 56:1221–1228, 2016. © 2016 Society of Plastics Engineers     

Preparation and properties of octadecylamine modified graphene oxide/styrene‐butadiene rubber composites through an improved melt compounding method

Octadecylamine modified graphene oxide/styrene‐butadiene rubber (GO‐ODA/SBR) composites are prepared by a novel and environmental‐friendly method called “Improved melt compounding”. A GO‐ODA/ethanol paste mixture is prepared firstly, and then blended with SBR by melt compounding. GO‐ODA sheets are uniformly dispersed in SBR as confirmed by scanning electron microscope, transmission electron microscopy, and X‐ray diffraction. The interfacial interaction between GO‐ODA and SBR is weaker than that between GO and SBR, which is proved by equilibrium swelling test and dynamic mechanical analysis. GO‐ODA/SBR show more pronounced “Payne effect” than GO/SBR composites, indicating enhanced filler networks resulted from the modification of GO with ODA. GO‐ODA/SBR composite has higher tensile strength and elongation at break than SBR and GO/SBR composite. The tensile strength and elongation at break for the composite with 5 parts GO‐ODA per hundred parts of rubber increase by 208% and 172% versus neat SBR, respectively. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 42907.     

Electrical conductivity and thermal properties of acrylonitrile‐butadiene‐styrene filled with multiwall carbon nanotubes

Composites of Acrylonitrile‐butadiene‐styrene (ABS) and multiwall carbon nanotubes (MWNTs) have been prepared via solution‐blending. The electrical conductivity of these composites is analyzed. The MWNT‐filled ABS shows percolation point of the electrical conductivity at low filler loadings (1–2 wt%). The micro‐structure of the composites is also analyzed by scanning electron microscopy showing that the nanotubes are dispersed quite homogeneously in the polymer‐matrix. The thermogravimetric analysis is used to study the thermal degradation of ABS/MWNTs composites in nitrogen. MWNTs tend to destabilize the ABS matrix in the 220–450°C degradation regions but improve the thermal stability in the 425–850°C regions. With further addition of MWNTs, the features of the destabilization in the 220–450°C degradation region did not change much but in the 425–850°C degradation process, the MWNTs reinforced stabilization and the quality of the char residue of amorphous carbon deposition was improved. POLYM. ENG. SCI., 2009. © 2009 Society of Plastics Engineers     

Preparation and characterization of epoxy resin modified with alkoxysilane‐ functionalized poly(urethane‐imide) by the sol–gel process

The sol–gel process has been frequently employed for preparation of high performance silica/polymer composites. In this paper, novel sol–gel precursor triethoxysilane‐terminated poly(urethane‐imide) (PUI‐Si), combining the advantages of polyurethane (PU) and polyimide, was synthesized and characterized. Then PUI‐Si was incorporated into the epoxy resin matrix to prepare a series of EP/PUI‐Si organic‐inorganic hybrids through an in situ sol–gel process and crosslinking reactions. The thermal stability of EP/PUI‐Si hybrids was evaluated by thermogravimetric analysis and the results show that the PUI‐Si could significantly improve the thermal properties of epoxy resin. The initial decomposition temperature of composites with 50 wt% PUI‐Si reached 347.1 °C, 157.3 °C higher than that of neat epoxy resin. Furthermore, the tensile strength and breaking elongation can also be clearly improved by adding a suitable amount of PUI‐Si. Similarly, the water contact angle increased to 97.4° with 70 wt% PUI‐Si, showing a hydrophobic surface. The morphology was investigated by transmission electron microscopy and the results reveal that the silica particles are smaller than 20 nm and have a strong interaction with the epoxy resin matrix, resulting in the above‐mentioned high performance properties. Copyright © 2011 Society of Chemical Industry     

Synthesis and properties of fluorinated graphene oxide bisphenol a epoxy nanocomposites

This study thoroughly studied the implements of fluorosilane modified graphene oxide (GO) on the mechanical, thermal, and water absorption properties of the epoxy composites built up by specific content of modified GO. Fluorosilane graphene oxide (GOSiF) was analyzed using Fourier transform infrared spectroscopy, thermogravimetric analysis, Raman spectroscopy, X‐ray photoelectron spectroscopy, and X‐ray diffractometer. The epoxy composites tensile and bending modulus were increased by 11.46% and 62.25% with 0.1 and 0.5 wt% GOSiF loading, respectively. The good interfacial interaction was observed between epoxy matrix and GOSiF nanosheets under scanning electron microscopy. The thermal stability increases with GOSiF loading. Epoxy composite with 0.3 wt% GOSiF shows 5 °C increases in the T_10%. The residual weight raised by 58.67% with 0.3 wt% GOSiF content. The water absorption study revealed small water uptake was obtained for all GOSiF composites. With 0.3 wt% loading of GOSiF, the maximum water content drops from 4.97% for neat epoxy to 1.98%. POLYM. ENG. SCI., 59:1250–1257 2019. © 2019 Society of Plastics Engineers     

Fabrication of surfactant‐removed polymer composites with single‐walled carbon nanotube networks

Polystyrene (PS) composites with a network of single‐walled carbon nanotubes (SWNTs) were fabricated by using monodispersed PS micospheres. First, PS spheres and surfactant‐dispersed SWNTs were mixed in water, then a hybrid cake was obtained by filtration via a microporous membrane and the SWNTs were filled within the spaces of packed polymer spheres. At this stage, the surfactants for dispersing SWNTs were totally removed from the composites by a thorough washing. Then the composite films with SWNT networks were obtained by compression molding at 160°C. Structure of the composites had been characterized by transmission electron microscopy and scanning electron microscopy. The present SWNT composites showed a low percolation threshold of electrical conductivities. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Mass‐produced graphene—HDPE nanocomposites: Thermal,rheological, electrical,and mechanical properties

Economically viable high‐density polyethylene (HDPE)/graphene nanocomposites were produced using mass produced graphene powder and an industrial twin‐screw melt‐compounding machine. Rheological and electrical properties were investigated and scanning electron microscopy was carried out to investigate graphene dispersion and its network formation in the matrix. Mechanical properties of the nanocomposites were evaluated using tensile, flexural and impact tests. Differential scanning calorimetry analysis indicated that the crystalline structure of the polymer might be affected by high loadings of graphene. SEM evaluation revealed reasonable graphene dispersion in the matrix. In addition, the amount of graphene required to form a percolated network was similar for both rheological and electrical networks. The nanocomposites exhibited a significant increase in Young's and flexural moduli without a notable reduction in impact strength up to 14 wt% graphene loading. In these experiments, compounding graphene powder with HDPE produced a clear and distinct improvement in mechanical properties at an industrially suitable low cost. POLYM. ENG. SCI., 59:675–682, 2019. © 2018 Society of Plastics Engineers     

Synergistic effect of three‐dimensional multi‐walled carbon nanotube–graphene nanofiller in enhancing the mechanical and thermal properties of high‐performance silicone rubber

The homogeneous dispersion of nanofillers and filler–matrix interfacial interactions are important factors in the development of high‐performance polymer materials for various applications. In the present work, a simple solution‐mixing method was used to prepare multi‐walled carbon nanotube (MWCNT)–graphene (G) (3:1, 1:1, 1:3) hybrids followed by their characterization through wide‐angle X‐ray diffraction, transmission electron microscopy and thermogravimetric analyses. Subsequently, MWCNT–G (1:1) hybrid was used as reinforcing filler in the formation of silicone rubber (VMQ) nanocomposites by solution intercalation, and their morphology and properties were investigated. Our findings showed that MWCNT–G (0.75 wt%)/VMQ composite exhibited significant improvements in tensile strength (110%) and Young's modulus (137%) compared to neat VMQ. The thermal stability of MWCNT–G (1 wt%)/VMQ was maximally improved by 154 °C compared to neat VMQ. Differential scanning calorimetry demonstrated the maximum improvement of glass transition temperature (4 °C), crystallization temperature (8 °C) and melting temperature (5 °C) for MWCNT–G (1 wt%)/VMQ nanocomposite with respect to neat VMQ. Swelling measurements confirmed that the crosslink density and solvent resistance were a maximum for hybrid nanocomposites. Such improvements in the properties of MWCNT–G/VMQ nanocomposites could be attributed to a synergistic effect of the hybrid filler. © 2013 Society of Chemical Industry     

Physico‐mechanical properties of nano‐polystyrene‐decorated graphene oxide–epoxy composites

Nano‐polystyrene (nPS)‐decorated graphene oxide (GO) hybrid nanostructures were successfully synthesized using stepwise microemulsion polymerization, and characterized using Fourier transform infrared (FTIR) spectroscopy, X‐ray diffraction (XRD), field‐emission scanning electron microscopy and transmission electron microscopy. XRD and FTIR spectra revealed the existence of a strong interaction between nPS and GO, which implied that the polymer chains were successfully grafted onto the surface of the GO. The nPS‐decorated GO hybrid nanostructures were compounded with epoxy using a hand lay‐up technique, and the effect of the nPS‐decorated GO on the mechanical, thermal and surface morphological properties of the epoxy matrix was investigated using a universal tensile machine, Izod impact tester, thermogravimetric analysis and contact angle measurements with a goniometer. It was observed that in the epoxy matrix, GO improved the compatibility. © 2017 Society of Chemical Industry     

Polystyrene/CaCO3 composites with different CaCO3 radius and different nano‐CaCO3 content—structure and properties

The Archimedes' principle and physical theory are attempted to analysis the densification and structure of the polystyrene (PS) composites by melt compounding with CaCO₃ having different particle size. The difference between the measured specific volume (ν) andthe theoretically calculated specific volume (ν_mix), Δν = ν−ν_mix, can reflect the densification of the composites. It is clearly demonstrated that the PS composites become more condensed with the reduction of the CaCO₃ particle size. Especially, when the content for nano‐CaCO₃ achieves 2 wt%, the Δν value of the composites reaches the least, which shows the best densification. Meanwhile, the glass transition temperature (T_g) reaches the maximum value of about 100°C by differential scanning calorimetry (DSC) and thermal mechanical analysis (TMA), which indirectly reveals the composites microstructure more condensed. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) reveal that 2 wt% nano‐CaCO₃ uniformly disperses in PS composites. The CaCO₃ selected in this experiment has certain toughening effect on PS. The impact and tensile strength increase with addition of nano‐CaCO₃, but the elongation at break decreases. When nano‐CaCO₃ content achieved 2 wt%, the impact and tensile strength present the maximum value of 1.63 KJ/m² and 44.5 MPa, which is higher than the pure PS and the composites filled with the same content of micro‐CaCO₃. POLYM. COMPOS., 31:1258–1264, 2010. © 2009 Society of Plastics Engineers     

Preparation of polyimide/siloxane‐functionalized graphene oxide composite films with high mechanical properties and thermal stability via in situ polymerization

An effective approach to prepare polyimide/siloxane‐functionalized graphene oxide composite films is reported. The siloxane‐functionalized graphene oxide was obtained by treating graphene oxide (GO) with 1,3‐bis(3‐aminopropyl)‐1,1,3,3‐tetra‐methyldisiloxane (DSX) to obtain DSX‐GO nanosheets, which provided a starting platform for in situ fabrication of the composites by grafting polyimide (PI) chains at the reactive sites of functional DSX‐GO nanosheets. DSX‐GO bonded with the PI matrix through amide linkage to form PI‐DSX‐GO films, in which DSX‐GO exhibited excellent dispersibility and compatibility. It is demonstrated that the obvious reinforcing effect of GO to PI in mechanical properties and thermal stability for PI‐DSX‐GO is obtained. The tensile strength of a composite film containing 1.0 wt% DSX‐GO was 2.8 times greater than that of neat PI films, and Young's modulus was 6.3 times than that of neat PI films. Furthermore, the decomposition temperature of the composite for 5% weight loss was approximately 30 °C higher than that of neat PI films. © 2015 Society of Chemical Industry     

Proanthocyanidin‐Induced Horizontal Arrangement in Poly(vinyl alcohol)/Graphene Composites with Enhanced Mechanical Properties

A green approach is employed to prepare mechanically enhanced composites by adding noncovalently proanthocyanidin (PC)‐modified graphene (PC‐rGO) into poly(vinyl alcohol) (PVA). Ascorbic acid (AA) is used as the reducing agent, and PC is used as a dispersant to synthesize low‐defect and fully dispersed graphene. After static treatment, the PC‐rGO sheets in the composite form a horizontally arranged structure. Compared with neat PVA, the Young's modulus of the graphene‐modified composites is significantly enhanced by approximately 79.3% with incorporation of 0.9 wt% PC‐rGO. The composites incorporated with GO or AA‐rGO (without PC) have randomly distributed GO structures and apparent rGO agglomeration, resulting in a weaker mechanical property. The dispersibility, degree of defects, distribution state of graphene, and interactions with the polymer matrix are directly related to the final mechanical performance. This new approach to mechanically enhance graphene‐embedded PVA composites provides the possibility for large‐scale production of graphene‐reinforced composite materials.     

Effect of curauá fiber content on the properties of poly(hydroxybutyrate‐co‐valerate) composites

Poly(hydroxybutyrate‐co‐valerate) (PHBV), a biodegradable polymer produced from a renewable microbiological source, was reinforced with varying amounts of curauá fibers (CFs). The composites were produced using a twin‐screw extrusion and injection process. Scanning electron microscopy showed poor adhesion between the matrix and fiber; however, mechanical testing showed that the addition of the fiber improved the mechanical properties. Composites with 20 and 30 wt% CF displayed the best properties; however, because of the difficulties in processing composites with a CF content of 30 wt%, it was concluded that the ideal content of CF was 20 wt%. POLYM. COMPOS., 2013. © 2013 Society of Plastics Engineers     

Preparation and characterization of covalently functionalized graphene using vinyl‐terminated benzoxazine monomer and associated nanocomposites with low coefficient of thermal expansion

We describe the preparation of vinyl‐terminated benzoxazine‐functionalized graphene using free radical grafting. The resulting functionalized graphene (f‐graphene) was incorporated into bis(3‐allyl‐3,4‐dihydro‐2H‐1,3‐benzoxazinyl)methane (V‐BF‐a) monomer in order that nanocomposites could be prepared. Results of scanning electron microscopy and transmission electron microscopy revealed that the sheets of f‐graphene were well dispersed throughout the matrix, and there was a strong interfacial interaction between the f‐graphene and polyV‐BF‐a. The inclusion of f‐graphene into the nanocomposites resulted in a material with a high thermal stability and a low coefficient of thermal expansion (CTE); increasing the content of f‐graphene reduced the CTE significantly more. A reduction in the CTE of up to 48% was produced by adding just 1 wt% of f‐graphene; this corresponded to an increase of 12 °C in the glass transition temperature. These results suggest that f‐graphene nanocomposites can be ‘tuned’ to give materials with both a low CTE and a high thermal stability, and that graphene composites of this type can thus be manufactured to withstand a wider range of temperatures.