Evolution of microstructure and mechanical properties of graphene oxide-reinforced aluminum alloy (6061) composite fabricated via accumulative roll bonding

Abstract

This study investigates the fabrication and characterization of Al alloy matrix composites reinforced with graphene oxide (GO) using accumulative roll bonding (ARB). The annealed Al 6061 sheets were processed through 5-pass ARB with GO reinforcement applied during the initial passes. Scanning electron microscopy revealed effective mitigation of GO agglomeration and improved interface bonding due to microscale material mixing. Raman spectroscopy confirmed the strong interaction between GO and the Al alloy matrix, as evidenced by the increased D band intensities and enhanced 2D band symmetry. Mechanical testing indicated an approximately 338.37% increase in yield strength (YS) and 86.42% improvement in hardness for the ARB-processed (ARBed) Al 6061/GO composite (0.2wt%) compared with annealed Al 6061 and an approximately 14.15% increase in YS and 17.23% improvement in hardness for the ARBed Al/GO composite (0.2wt%) compared with unreinforced ARBed Al 6061 specimens after five passes. X-ray diffraction analysis indicated an increased dislocation density, corroborating the observed enhancements in mechanical properties. Fracture surface analysis revealed reduced elongation with deep dimples, highlighting the tradeoff between strength and ductility. These results demonstrate the effectiveness of ARB for integrating GO into the Al 6061 matrix to improve the mechanical performance and interfacial bonding and underscore its potential for advanced composite materials.

Keywords

severe plastic deformation / accumulative roll bonding / aluminum matrix composite / Al 6061 / graphene oxide / fractography

References

[1] Rawal SP. Metal-matrix composites for space applications. JOM. 2001, 53414.

[2] Prasad SV, Asthana R. Aluminum metal-matrix composites for automotive applications: Tribological considerations. Tribol. Lett.. 2004, 173445.

[3] Lloyd DJ. Particle reinforced aluminium and magnesium matrix composites. Int. Mater. Rev.. 1994, 3911.

[4] V. Pandey, R. Seetharam, and H. Chelladurai, A comprehensive review: Discussed the effect of high-entropy alloys as reinforcement on metal matrix composite properties, fabrication techniques, and applications, J. Alloy. Compd., 1002(2024), art. No. 175095.

[5] Pandey V, Choudhary T, Bajpai Aet al. . Verma P, Samuel OD, Verma TNet al. . Microstructure tribological characterization of copper metal matrix reinforced with cerium oxide. Advancement in Materials, Manufacturing and Energy Engineering, Vol. II. 2022, Singapore, Springer273.

[6] H.R. Jafarian, M.M. Mahdavian, S.A.A. Shams, and A.R. Eivani, Microstructure analysis and observation of peculiar mechanical properties of Al/Cu/Zn/Ni multi-layered composite produced by accumulative-roll-bonding (ARB), Mater. Sci. Eng. A, 805(2021), art. No. 140556.

[7] Jamaati R, Toroghinejad MR. High-strength and highly-uniform composite produced by anodizing and accumulative roll bonding processes. Mater. Des.. 2010, 31104816.

[8] Ferreira F, Ferreira I, Camacho E, Lopes F, Marques AC, Velhinho A. Graphene oxide-reinforced aluminium-matrix nanostructured composites fabricated by accumulative roll bonding. Composites, Part B. 2019, 164265.

[9] Ahmadi Ana SV, Reihanian M, Lotfi B. Accumulative roll bonding (ARB) of the composite coated strips to fabricate multi-component Al-based metal matrix composites. Mater. Sci. Eng. A. 2015, 647303.

[10] Valiev RZ, Langdon TG. Principles of equal-channel angular pressing as a processing tool for grain refinement. Prog. Mater. Sci.. 2006, 517881.

[11] Saito Y, Utsunomiya H, Tsuji N, Sakai T. Novel ultra-high straining process for bulk materials—development of the accumulative roll-bonding (ARB) process. Acta Mater.. 1999, 472579.

[12] Navid MNF, Hamed M, Mohammad R, Jose-Maria C. Accumulative roll bonding of aluminum/stainless steel sheets. J. Ultrafine Grained Nanostruct. Mater.. 2017, 5011

[13] Tsuji N, Ito Y, Saito Y, Minamino Y. Strength and ductility of ultrafine grained aluminum and iron produced by ARB and annealing. Scripta Mater.. 2002, 4712893.

[14] J.K. Tiwari, A. Mandal, N. Sathish, V.A.N. Ch, and A.K. Srivastava, Graphene platelets reinforced aluminum matrix composite with enhanced strength by hot accumulative roll bonding, (2018), arXiv: 1807.00198.10.48550/arXiv: 1807.00198. https://doi.org/10.48550/arXiv.1807.00198.

[15] Eivani AR, Shojaei A, Salehi MT, Jafarian HR, Park N. On the evolution of microstructure and fracture behavior of multilayered copper sheet fabricated by accumulative roll bonding. J. Mater. Res. Technol.. 2021, 10291.

[16] Li BL, Tsuji N, Kamikawa N. Microstructure homogeneity in various metallic materials heavily deformed by accumulative roll-bonding. Mater. Sci. Eng. A. 2006, 4231–2331.

[17] Reihanian M, Hadadian FK, Paydar MH. Fabrication of Al–2vol% Al₂O₃/SiC hybrid composite via accumulative roll bonding (ARB): An investigation of the microstructure and mechanical properties. Mater. Sci. Eng. A. 2014, 607188.

[18] Reihanian M, Bagherpour E, Paydar MH. On the achievement of uniform particle distribution in metal matrix composites fabricated by accumulative roll bonding. Mater. Lett.. 2013, 9159.

[19] Reihanian M, Bagherpour E, Paydar MH. Particle distribution in metal matrix composites fabricated by accumulative roll bonding. Mater. Sci. Technol.. 2012, 281103.

[20] Reihanian M, Jalili Shahmansouri M, Khorasanian M. High strength Al with uniformly distributed Al₂O₃ fragments fabricated by accumulative roll bonding and plasma electrolytic oxidation. Mater. Sci. Eng. A. 2015, 640195.

[21] Balandin AA. Thermal properties of graphene and nanostructured carbon materials. Nat. Mater.. 2011, 108569.

[22] Lee CG, Wei XD, Kysar JW, Hone J. Measurement of the elastic properties and intrinsic strength of monolayer graphene. Science. 2008, 3215887385.

[23] Novoselov KS, Geim AK, Morozov SVet al. . Electric field effect in atomically thin carbon films. Science. 2004, 3065696666.

[24] Yan SJ, Dai SL, Zhang XYet al. . Investigating aluminum alloy reinforced by graphene nanoflakes. Mater. Sci. Eng. A. 2014, 612440.

[25] Wang JY, Li ZQ, Fan GL, Pan HH, Chen ZX, Zhang D. Reinforcement with graphene nanosheets in aluminum matrix composites. Scripta Mater.. 2012, 668594.

[26] Bisht A, Srivastava M, Kumar RM, Lahiri I, Lahiri D. Strengthening mechanism in graphene nanoplatelets reinforced aluminum composite fabricated through spark plasma sintering. Mater. Sci. Eng. A. 2017, 69520.

[27] Li JL, Xiong YC, Wang XDet al. . Microstructure and tensile properties of bulk nanostructured aluminum/graphene composites prepared via cryomilling. Mater. Sci. Eng. A. 2015, 626400.

[28] Jeon CH, Jeong YH, Seo JJet al. . Material properties of graphene/aluminum metal matrix composites fabricated by friction stir processing. Int. J. Precis. Eng. Manuf.. 2014, 1561235.

[29] V. Pandey, R. Seetharam, H. Chelladurai, and J. Immanuel R, Fabrication and characterization of Al alloy composites reinforced with nanocrystalline Al₄CrFeMnTi_0.25 high-entropy alloy particles via double ultrasonic stir casting for aerospace applications, J. Alloy. Compd., 1010(2025), art. No. 177900.

[30] Saboori A, Pavese M, Badini C, Fino P. Microstructure and thermal conductivity of Al–graphene composites fabricated by powder metallurgy and hot rolling techniques. Acta Metall. Sin. Engl. Lett.. 2017, 307675.

[31] Salimi S, Izadi H, Gerlich AP. Fabrication of an aluminum-carbon nanotube metal matrix composite by accumulative roll-bonding. J. Mater. Sci.. 2011, 462409.

[32] Yao GC, Mei QS, Li JYet al. . Cu/C composites with a good combination of hardness and electrical conductivity fabricated from Cu and graphite by accumulative roll-bonding. Mater. Des.. 2016, 110124.

[33] Liu XR, Wei DJ, Zhuang LM, Cai C, Zhao YH. Fabrication of high-strength graphene nanosheets/Cu composites by accumulative roll bonding. Mater. Sci. Eng. A. 2015, 6421.

[34] Vaidyanath LR, Nicholas MG, Milner DR. Pressure welding by rolling. British Welding J.. 1959, 613

[35] Dasari BL, Morshed M, Nouri JM, Brabazon D, Naher S. Mechanical properties of graphene oxide reinforced aluminium matrix composites. Composites, Part B. 2018, 145136.

[36] Zaaba NI, Foo KL, Hashim U, Tan SJ, Liu WW, Voon CH. Synthesis of graphene oxide using modified hummers method: Solvent influence. Procedia Eng.. 2017, 184469.

[37] Liu JH, Khan U, Coleman Jet al. . Graphene oxide and graphene nanosheet reinforced aluminium matrix composites: Powder synthesis and prepared composite characteristics. Mater. Des.. 2016, 9487.

[38] Ashwath P, Jeyapandiarajan P, Joel Jet al. . Flexural studies of graphene reinforced aluminium metal matrix composite. Mater. Today Proc.. 2018, 5513459.

[39] Tian WM, Li SM, Wang B, Chen X, Liu JH, Yu M. Graphene-reinforced aluminum matrix composites prepared by spark plasma sintering. Int. J. Miner. Metall. Mater.. 2016, 236723.

[40] Dixit S, Mahata A, Mahapatra DR, Kailas SV, Chattopadhyay K. Multi-layer graphene reinforced aluminum-manufacturing of high strength composite by friction stir alloying. Composites, Part B. 2018, 13663.

[41] L. Chen, Z.C. Li, S.J. Yan, H.B. Luo, X.W. Li, and A.X. Sha, Enhanced mechanical properties of graphene oxide reinforced aluminum with lamellar microstructure and crystallographic alignment, Carbon, 245(2025), art. No. 120792.

[42] J.K. Tiwari, A. Mandal, A. Rudra, N. Sathish, S. Kumar, and A.K. Singh, Influence of graphene content on the mechanical properties of severely deformed graphene/aluminum composite, Mater. Chem. Phys., 248(2020), art. No. 122939.

[43] Faria P, Duarte P, Barbosa D, Ferreira I. New composite of natural hydraulic lime mortar with graphene oxide. Constr. Build. Mater.. 2017, 1561150.

[44] N. Méndez-Lozano, F. Pérez-Reynoso, and C. González-Gutiérrez, Eco-friendly approach for graphene oxide synthesis by modified hummers method, Materials, 15(2022), No. 20, art. No. 7228.

[45] Alam SN, Sharma N, Kumar L. Synthesis of graphene oxide (GO) by modified hummers method and its thermal reduction to obtain reduced graphene oxide (rGO). Graphene. 2017, 611.

[46] S. Kumar, R. Sehgal, M.F. Wani, M.D. Sharma, U. Ziyamukhamedova, and T. Ahmad Dar, Next-generation eco-friendly MR fluid: Hybrid GO/Fe₂O₃ encapsulated carbonyl iron microparticles with improved magnetorheological, tribological, and corrosion resistance properties, Carbon, 214(2023), art. No. 118331.

[47] H.T. Yu, B.W. Zhang, C. Bulin, R.H. Li, and R.G. Xing, High-efficient synthesis of graphene oxide based on improved hummers method, Sci. Rep., 6(2016), art. No. 36143.

[48] Tiwari JK, Mandal A, Rudra A, Mukherjee D, Sathish N. Evaluation of mechanical and thermal properties of bilayer graphene reinforced aluminum matrix composite produced by hot accumulative roll bonding. J. Alloy. Compd.. 2019, 80149.

[49] Liu WC, Ke YJ, Sugio Ket al. . Microstructure of commercial-purity aluminum sheets processed by accumulative roll bonding (ARB) at a series of cyclic preheating conditions. Trans. Indian Inst. Met.. 2022, 7592335.

[50] Dehghan M, Qods F, Gerdooei M, Mohammadian-Semnani H. Influence of intermediate heating in cross accumulative roll-bonding process on planar isotropy of the mechanical properties of commercial purity aluminium sheet. Met. Mater. Int.. 2021, 27124937.

[51] Cheng KY, Tieu K, Lu C, Zhu HT, Pei LQ. Effect of pre-heating on the microstructural evolution and super-plasticity of Al deformed by accumulative roll bonding. Steel Res. Int.. 2013, 84121209.

[52] Md Ali A, Omar MZ, Hashim H, Salleh MS, Mohamed IF. Recent development in graphene-reinforced aluminium matrix composite: A review. Rev. Adv. Mater. Sci.. 2021, 601801.

[53] Huang F, Tao NR. Effects of strain rate and deformation temperature on microstructures and hardness in plastically deformed pure aluminum. J. Mater. Sci. Technol.. 2011, 2711.

[54] Singh VP, Gupta GK, Mishra S. Microstructural evolution and mechanical properties of multi-layered aluminum alloy 6061 processed by accumulative roll bonding. J. Mater. Eng. Perform.. 2025, 3486828.

[55] H.D. Wang, H.T. Zheng, M.S. Hu, Z.L. Ma, and H. Liu, Synergistic effect of Al₂O₃-decorated reduced graphene oxide on microstructure and mechanical properties of 6061 aluminium alloy, Sci. Rep., 14(2024), No. 1, art. No. 16213.

[56] X.L. Zou, Z.J. Cheng, Y. Yan, Microstructure, mechanical properties and interfacial features of graphene oxide reinforced 7075 composites fabricated by ultrasonic assisted casting, J. Alloy. Compd., 1003(2024), art. No. 175505.

[57] Patidar S, Tiwari JK, Das Aet al. . Study on microstructure and tribological behavior of additively manufactured graphene/AlSi₁₀Mg composite. J. Mater. Eng. Perform.. 2024, 332212503.

[58] Uppada S, Yanda S, Kandi KK, Prakash P, Janaki DV. Effect of accumulative roll bonding on microstructure and mechanical behavior of Al6061. J. Inst. Eng. India Ser. D. 2025, 1061599.

[59] Ö. Laçin, Yeni bir yaklaşımla elde edilen grafen oksit sentezlerinde SEM ve TEM analizleri, Avrupa Bilim ve Teknoloji Dergisi, (2022), No. 39, p. 76.

[60] Guliyeva NA, Abaszade RG, Khanmammadova EA, Azizov EM. Synthesis and analysis of nanostructured graphene oxide. J. Optoelectron. Biomed. Mater.. 2023, 15123.

[61] Lee SH, Saito Y, Sakai T, Utsunomiya H. Microstructures and mechanical properties of 6061 aluminum alloy processed by accumulative roll-bonding. Mater. Sci. Eng. A. 2002, 3251–2228.

[62] Ou L, Li LY, Fan CH, Nie YF, Yang JJ. Enhancement of strength and ductility in 6061Al alloy processed by cross accumulative roll bonding. Trans. Nonferrous Met. Soc. China. 2023, 3372001.

[63] Feng ZQ, Yang YQ, Chen YXet al. . In-situ TEM investigation of fracture process in an Al–Cu–Mg alloy. Mater. Sci. Eng. A. 2013, 586259.

[64] Rezaei MR, Toroghinezhad M, Ashrafizadeh F. Analysis of strengthening mechanisms in an artificially aged ultrafine grain 6061 aluminum alloy. J. Ultrafine Grained Nanostruct. Mater.. 2017, 502152

[65] Klinger M. More features, more tools, more CrysTBox. J. Appl. Crystallogr.. 2017, 5041226.

[66] Klinger M, Jäger A. Crystallographic Tool Box (CrysT-Box): Automated tools for transmission electron microscopists and crystallographers. J. Appl. Crystallogr.. 2015, 4862012.

[67] Palei BB, Dash T, Biswal SK. Graphene reinforced aluminum nanocomposites: Synthesis, characterization and properties. J. Mater. Sci.. 2022, 57188544.

[68] Farhadipour P, Sedighi M, Vini MH. Using warm accumulative roll bonding method to produce Al–Al₂O₃ metal matrix composite. Proc. Inst. Mech. Eng., Part B: J. Eng. Manuf.. 2017, 2315889.

[69] Humphreys FJ, Hatherly M. Recrystallization textures. Recrystallization and Related Annealing Phenomena. 20042nd ed.Amsterdam, Elsevier379.

RIGHTS & PERMISSIONS

University of Science and Technology Beijing