In this work graphene nanoplatelets (GNPs) and micrometric carbon fibres (CFs) have been added to an epoxy resin for producing high performance composite materials. Rheological analysis indicates that CFs slightly increase viscosity without altering the Newtonian behavior of the epoxy resin, while GNPs significantly increase viscosity due to filler-polymer interactions, shifting the behavior to shear-thinning. The produced composite present improved stiffness and strength, with flexural strength increasing from 77 MPa (neat epoxy) to 120 MPa and the elastic modulus rising from 2.2 GPa to 20 GPa in reinforced samples without changing the glass transition temperature (Tg = 170°C). Adding the fillers, the thermal conductivity increases by 220% and a resistivity of 670 Ω cm is reached in the best performing system. The combination of hybrid fillers enables synergistic reinforcement, making the epoxy composites suitable for advanced structural and thermal management applications.
KatariMKrishnamoorthyGJeyaramanJ. Novel materials and processes for miniaturization in semiconductor packaging. J Artif Intell Gen Sci2024; 2: 251–271.
2.
KNRoutCS. Conducting polymers: a comprehensive review on recent advances in synthesis, properties and applications. RSC Adv2021; 11: 5659–5697.
3.
PugliaDValentiniLKennyJM. Analysis of the cure reaction of carbon nanotubes/epoxy resin composites through thermal analysis and Raman spectroscopy. J Appl Polym Sci2003; 88: 452–458.
4.
HeinleCDrummerD. Potential of thermally conductive polymers for the cooling of mechatronic parts. Phys Procedia2010; 5: 735–744.
5.
BoschettoGCarapezziSTodri-SanialA. Graphene and carbon nanotubes for electronics nanopackaging. IEEE Open J Nanotechnol2021; 2: 120–128.
6.
ColemanJNKhanUBlauWJ, et al.Small but strong: a review of the mechanical properties of carbon nanotube–polymer composites. Carbon N Y2006; 44: 1624–1652.
7.
Laborde-LahozPMaserWMartínezT, et al.Mechanical characterization of carbon nanotube composite materials. Mech Adv Mater Struct2005; 12: 13–19.
8.
JiXXuYZhangW, et al.Review of functionalization, structure and properties of graphene/polymer composite fibers. Compos Part A Appl Sci Manuf2016; 87: 29–45.
9.
ProlongoSGJimenez-SuarezAMoricheR, et al.In situ processing of epoxy composites reinforced with graphene nanoplatelets. Compos Sci Technol2013; 86: 185–191.
10.
LiWDichiaraABaiJ. Carbon nanotube–graphene nanoplatelet hybrids as high-performance multifunctional reinforcements in epoxy composites. Compos Sci Technol2013; 74: 221–227.
11.
PANaina MohamedSSingaraveluDL, et al.A review on graphene/graphene oxide supported electrodes for microbial fuel cell applications: challenges and prospects. Chemosphere2022; 296: 133983.
12.
ImHKimJ. Thermal conductivity of a graphene oxide–carbon nanotube hybrid/epoxy composite. Carbon N Y2012; 50: 5429–5440.
13.
WangFDrzalLTQinY, et al.Mechanical properties and thermal conductivity of graphene nanoplatelet/epoxy composites. J Mater Sci2015; 50: 1082–1093.
14.
BilisikKAkterM. Polymer nanocomposites based on graphite nanoplatelets (GNPs): a review on thermal-electrical conductivity, mechanical and barrier properties. J Mater Sci2022; 57: 7425–7480.
15.
LiFWangHKeY, et al.Preparation of GNP/SBR thermal conductivity composites with high strength and toughness by synergistic construction of interfacial multiple non-covalent and covalent bonds. Polym Compos2024; 45: 5633–5642.
16.
WangZYangQZhengX, et al.Fused deposition modeling of isotactic polypropylene/graphene nanoplatelets composites: achieving enhanced thermal conductivity through filler orientation. Polymers (Basel)2024; 16: 772.
17.
GuJYangXLvZ, et al.Functionalized graphite nanoplatelets/epoxy resin nanocomposites with high thermal conductivity. Int J Heat Mass Transf2016; 92: 15–22.
18.
CaiLAl-OstazALiX, et al.Processing and mechanical properties investigation of epoxy-impregnated graphene paper. J Nanomech Micromech2016; 6: 04016005.
19.
YangS-YLinW-NHuangY-L, et al.Synergetic effects of graphene platelets and carbon nanotubes on the mechanical and thermal properties of epoxy composites. Carbon N Y2011; 49: 793–803.
20.
ZaldivarRJNokesJPKimHI. The effect of surface treatment on graphite nanoplatelets used in fiber reinforced composites. J Appl Polym Sci2014; 131: app.39994.
21.
LaLBTNguyenHTranLC, et al.Exfoliation and dispersion of graphene nanoplatelets for epoxy nanocomposites. Adv Nanocompos2024; 1: 39–51.
22.
BragagliaMPaleariLLamastraFR, et al.Graphene nanoplatelet, multiwall carbon nanotube, and hybrid multiwall carbon nanotube–graphene nanoplatelet epoxy nanocomposites as strain sensing coatings. J Reinf Plast Compos2021; 40: 632–643.
23.
PedrazzoliDPegorettiAKalaitzidouK. Synergistic effect of exfoliated graphite nanoplatelets and short glass fiber on the mechanical and interfacial properties of epoxy composites. Compos Sci Technol2014; 98: 15–21.
24.
OwaisMZhaoJImaniA, et al.Synergetic effect of hybrid fillers of boron nitride, graphene nanoplatelets, and short carbon fibers for enhanced thermal conductivity and electrical resistivity of epoxy nanocomposites. Compos Part A Appl Sci Manuf2019; 117: 11–22.
25.
HuXWangLXuF, et al.In situ observations of fractures in short carbon fiber/epoxy composites. Carbon N Y2014; 67: 368–376.
26.
CapelaCOliveiraSEFerreiraJAM. Fatigue behavior of short carbon fiber reinforced epoxy composites. Compos Part B Eng2019; 164: 191–197.
27.
ChenQWuFJiangZ, et al.Improved interlaminar fracture toughness of carbon fiber/epoxy composites by a combination of extrinsic and intrinsic multiscale toughening mechanisms. Compos Part B Eng2023; 252: 110503.
28.
SharmaHKumarARanaS, et al.An overview on carbon fiber-reinforced epoxy composites: effect of graphene oxide incorporation on composites performance. Polymers (Basel)2022; 14: 1548.
29.
BragagliaMLamastraFRTuluiM, et al.Low temperature sputtered ITO on glass and epoxy resin substrates: influence of process parameters and substrate roughness on morphological and electrical properties. Surf Interfaces2019; 17: 1–7.
30.
GuerraVWanCDegirmenciV, et al.2D boron nitride nanosheets (BNNS) prepared by high-pressure homogenisation: structure and morphology. Nanoscale2018; 10: 19469–19477.
31.
PullicinoEZouWGresilM, et al.The effect of shear mixing speed and time on the mechanical properties of GNP/epoxy composites. Appl Compos Mater2017; 24: 301–311.
32.
ZhangZTanYFengK, et al.Effect of hyperbranched epoxy resin on mechanical properties of short carbon fiber-reinforced epoxy composites. Polym Compos2016; 37: 2727–2733.
33.
KhunNWZhangHLimLH, et al.Tribological properties of short carbon fibers reinforced epoxy composites. Friction2014; 2: 226–239.
34.
BragagliaMPaleariLMarianiM, et al.Sustainable formaldehyde-free copper electroless plating on carbon-epoxy substrates. J Mater Sci Mater Electron2024; 35: 707.
35.
van der PauwLJ. A method of measuring specific resistivity and HALL effect of discs of arbitrary shape. In: Semicond. Devices pioneer. Pap. World Scientific, 1991, pp. 174–182.
36.
ChouganMMarottaELamastraFR, et al.High performance cementitious nanocomposites: the effectiveness of nano-Graphite (nG). Constr Build Mater2020; 259: 119687.
37.
LiWDichiaraABaiJ. Carbon nanotube-graphene nanoplatelet hybrids as high-performance multifunctional reinforcements in epoxy composites. Compos Sci Technol2013; 74: 221–227.
38.
YuanGLiBLiX, et al.Effect of liquid crystalline texture of mesophase pitches on the structure and property of large-diameter carbon fibers. ACS Omega2019; 4: 1095–1102.
39.
PopovaAN. Crystallographic analysis of graphite by X-Ray diffraction. Coke Chem2017; 60: 361–365.
40.
JiangGPickeringSJ. Structure–property relationship of recycled carbon fibres revealed by pyrolysis recycling process. J Mater Sci2016; 51: 1949–1958.
41.
Matielli RodriguesGGFaulstich de PaivaJMBraga do CarmoJ, et al.Recycling of carbon fibers inserted in composite of DGEBA epoxy matrix by thermal degradation. Polym Degrad Stab2014; 109: 50–58.
42.
ShteinMPri-BarIVarenikM, et al.Characterization of graphene-nanoplatelets structure via thermogravimetry. Anal Chem2015; 87: 4076–4080.
43.
SongYZhengQ. A guide for hydrodynamic reinforcement effect in nanoparticle-filled polymers. Crit Rev Solid State Mater Sci2016; 41: 318–346.
44.
EinsteinA. On the motion of small particles suspended in liquids at rest required by the molecular-kinetic theory of heat. Ann Phys1905; 17: 549–560.
45.
NadivRFernandesRMFOchbaumG, et al.Polymer nanocomposites: insights on rheology, percolation and molecular mobility. Polymer2018; 153: 52–60.
46.
GenoveseDB. Shear rheology of hard-sphere, dispersed, and aggregated suspensions, and filler-matrix composites. Adv Colloid Interface Sci2012; 171–172: 1–16.
47.
SongYZhengQ. Concepts and conflicts in nanoparticles reinforcement to polymers beyond hydrodynamics. Prog Mater Sci2016; 84: 1–58.
48.
KimJASeongDGKangTJ, et al.Effects of surface modification on rheological and mechanical properties of CNT/epoxy composites. Carbon N Y2006; 44: 1898–1905.
49.
PolychronopoulosNDVlachopoulosJ. Polymer processing and rheology. In: Jafar MazumderMASheardownHAl-AhmedA (eds). Funct Polym. Cham: Springer International Publishing, 2018, pp. 1–47.
50.
LinXZhangKLiK, et al.Dependence of rheological behaviors of polymeric composites on the morphological structure of carbonaceous nanoparticles. J Appl Polym Sci2018; 135: 46416.
51.
LiBZhongWH. Review on polymer/graphite nanoplatelet nanocomposites. J Mater Sci2011; 46: 5595–5614.
52.
NgoT-DTon-ThatM-THoaSV, et al.Effect of temperature, duration and speed of pre-mixing on the dispersion of clay/epoxy nanocomposites. Compos Sci Technol2009; 69: 1831–1840.
53.
HsuehC. Effects of aspect ratios of ellipsoidal inclusions on elastic stress transfer of ceramic composites. J Am Ceram Soc1989; 72: 344–347.
54.
FuSFengXLaukeB, et al.Effects of particle size, particle/matrix interface adhesion and particle loading on mechanical properties of particulate – polymer composites. Compos Part B2008; 39: 933–961.
55.
KuoMCTsaiCMHuangJC, et al.PEEK composites reinforced by nano-sized SiO2 and Al2O3 particulates. Mater Chem Phys2005; 90: 185–195.
56.
SaitoSSatoSAraoY. The effect of processing/curing temperature and viscosity of epoxy resins on the flexural/tensile properties of GNP-epoxy resin nanocomposites. Compos Part A Appl Sci Manuf2024; 183: 108222.
57.
ZhuYSuLDengJ, et al.Impact of GNP content on cure behaviors and diverse properties of epoxy composites modified with graphene nanoplatelets: a comprehensive study. Mater Today Commun2023; 37: 107014.
58.
FuGHuoDShyhaI, et al.Machinability investigation of polymer/GNP nanocomposites in micro-milling. Int J Adv Manuf Technol2022; 119: 2341–2353.
59.
ChandrasekaranSSatoNTölleF, et al.Fracture toughness and failure mechanism of graphene based epoxy composites. Compos Sci Technol2014; 97: 90–99.
60.
HongJYoonSHwangT, et al.High thermal conductivity epoxy composites with bimodal distribution of aluminum nitride and boron nitride fillers. Thermochim Acta2012; 537: 70–75.
61.
GuerraVWanCMcNallyT. Thermal conductivity of 2D nano-structured boron nitride (BN) and its composites with polymers. Prog Mater Sci2019; 100: 170–186.
62.
BalbergI. A comprehensive picture of the electrical phenomena in carbon black–polymer composites. Carbon N Y2002; 40: 139–143.
63.
BundeADieterichW. Percolation in composites. J Electroceram2000; 5: 81–92.
TianchenYJianYRuigangS, et al.A geometric percolation model for non-spherical excluded volumes. J Phys D Appl Phys2003; 36: 738.
66.
JangDYoonHNNamIW, et al.Effect of carbonyl iron powder incorporation on the piezoresistive sensing characteristics of CNT-based polymeric sensor. Compos Struct2020; 244: 112260.
67.
DuFFischerJEWineyKI. Effect of nanotube alignment on percolation conductivity in carbon nanotube/polymer composites. Phys Rev B2005; 72: 121404.
68.
AguilarJOBautista-QuijanoJRAvilesF. Influence of carbon nanotube clustering on the electrical conductivity of polymer composite films. Express Polym Lett2010; 4: 292–299.
69.
KovacsJZVelagalaBSSchulteK, et al.Two percolation thresholds in carbon nanotube epoxy composites. Compos Sci Technol2007; 67: 922–928.
70.
HuNMasudaZYanC, et al.The electrical properties of polymer nanocomposites with carbon nanotube fillers. Nanotechnology2008; 19: 215701.
71.
GongSCuiWZhangQ, et al.Integrated ternary bioinspired nanocomposites via synergistic toughening of reduced graphene oxide and double-walled carbon nanotubes. ACS Nano2015; 9: 11568–11573.
72.
ScaffaroRMaioA. Integrated ternary bionanocomposites with superior mechanical performance via the synergistic role of graphene and plasma treated carbon nanotubes. Compos Part B Eng2019; 168: 550–559.
