Synthesis, Characterization, and Electrochemical Performance of Reduced Graphene Oxide-Metal (Cu,Zn)-Oxide Materials

Sugianto Sugianto, Ngurah Made Dharma Putra, Endah F. Rahayu, Wahyu B. Widayatno, Cherly Firdharini, Slamet Priyono, Didik Aryanto


The reduced graphene oxide (rGO) and metal (Cu,Zn)-oxide composites were prepared using a one-step hydrothermal technique. The role of (Cu,Zn)-oxide on the physical and electrochemical properties of the composite was investigated. The composite consists of various shapes of ZnO nanoflowers and micro-spheres, as well as Cu-oxide nanoflakes and octahedron-like shapes. The (Cu,Zn)-oxides were formed in between the rGO layers and observed in the rGO-ZnO, rGO-CuO, and rGO-CuO-ZnO composites. The presence of ZnO, CuO, and rGO within the composite structure is also confirmed by the analyses of crystal structure, microstructure, and surface functional groups. Some excess impurities remaining from the surfactant give considerable differences in the electrochemical performance of the composites. The specific capacitance values of the rGO, rGO-ZnO, rGO-CuO, rGO-(0.5CuO-0.5ZnO), and rGO-(0.25CuO-0.75ZnO) composites are 9.32, 58.53, 54.14, 25.21, and 69.27 F/g, respectively. The formation ofa double metal-oxide structure as well as their insertion into the rGO sheet can significantly improve the electrochemical properties of the supercapacitor.


Composite; Cu-oxide, Morphology; Reduced graphene oxide (rGO); Zinc oxide (ZnO)

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Alajlani, Y., Placido, F., Chu, H. O., Bold, R. D., Fleming, L., and Gibson, D. (2017). Characterisation of Cu2O/CuO thin films produced by plasma-assisted DC sputtering for solar cell application. Thin Solid Films, 642, 45-50.

Alver, U., Tanriverdi, A., and Akgul, O. (2016). Hydrothermal preparation of ZnO electrodes synthesized from different precursors for electrochemical supercapacitors. Synthetic Metals, 211, 30-34.

Aravinda L.S., Udaya Bhat K., and Ramachandra Bhat B. (2013). Nano CeO2/activated carbon based composite electrodes for high performance supercapacitor. Materials Letters, 112, 158-161.

Bian, H.Q., Ma, S.Y., Li, F.M., and Zhu, H.B. (2013). Influence of ZnO buffer layer on microstructure and raman scattering of ZnO:Ag film on Si substrate. Superlattice and Microstructures, 58, 171-177.

Boukhoubza, I., Khenfounch, M., Achehboune, M., Leontie, L., Carlescu, A., Doroftei, C., Mothudi, B.M., Zorkani, I., and Jorio, A. (2020). Graphene oxide coated flower-shaped ZnO nanorods: Optoelectronic properties. Journal Alloys and Compounds, 831, 154874.

Bundesmann, C., Askenov, N., Schubert, M., Spemann, D., Butz, T., Kaidashev, E.M., Lorenz, M., & Grundmann, M. (2003). Raman scattering in ZnO thin films doped with Fe, Sb, Al, Ga and Li. Applied Physics Letters, 83, 974-1976.

Chen, K., and Xue, D. (2014). Reaction route to the crystallization of copper oxides. Applied Science and Convergence Technology, 23, 14-26.

Cheng, W., He, H., Liu, X., Liu, Y., Zhang, Z., Li, S., Zhang, R., Wang, X., Wu, Z., and Wu, Z. (2021). The study on nanostructural evolution of CuO/Graphene oxide nanocomposite during the first discharge processes. Materials Chemistry and Physics, 260, 124157.

Dar, R. A., Naikoo, G. A., Srivastava, A. K., Hassan, I. U., Karna, S. P., Giri, L., Shaikh, A. M. H., Rezakazemi, M., and Ahmed, W. (2022). Performance of graphene‑zinc oxide nanocomposite coated‑glassy carbon electrode in the sensitive determination of para‑nitrophenol. Scientific Reports, 12, 1-14.

Daraghmeh, A., Hussain, S., Saadeddin, I., servera, L., Xuriguera, E., Cornet, A., and Ciera, A. (2017). A study of carbon nanofibers and active carbon as symmetric supercapasitor in aqueous electrolyte: A comparative study. Nanoscale Research Letters, 12(1), 1-10.

Debbichi, L., Marco de Lucas, M. C., Pierson, J. F., and Krüger, P. (2012). Vibrational properties of CuO and Cu4O3 from first-principles calculations, and raman and infrared spectroscopy. The Journal Physical Chemistry C, 116, 10232-10237.

Dong S., Chen X., Zhang X., and Cui G. (2013). Nanostructured transition metal nitrides for energy storage and fuel cells. Coordination Chemistry Reviews, 257(13–14), 1946-1956.

Du, X., Wang, S., Liu, Y., Lu, M., Wu, K., Lu, M. (2019). Self-assembly of free-standing hybrid film based on graphene and zinc oxide nanoflakes for high-performance supercapacitors. Journal of Solid State Chemistry, 277, 441-447.

Faraji, S., and Ani, F.N. (2015). The development supercapacitor from activated carbon by electroless plating-a review. Renewable and Sustainable Energy Reviews, 42, 823-834.

Firoz B. K., Siva S.S.P., Anbu K.M. 2013. Functionalisation of fabrics with conducting polymer for tuning capacitance and fabrication of supercapacitor. Carbohydrate Polymers, 94, 487–495.

Ghenaatian H.R., Mousavi M.F., and Rahmanifar M.S. (2012). High performance hybrid supercapacitor based on two nanostructured conducting polymers: Selfdoped polyaniline and polypyrrole nanofibers. Electrochimica Acta, 78, 212-22.

Kalaiarasi, J., Pragathiswaran, C., and Subramani, P. (2021) Green chemistry approach for the functionalization of reduced graphene and ZnO as efficient supercapacitor application. Journal of Molecular Structure, 1242, 130704.

Kim, D., and Leem, J.‑Y. (2021). Optimal temperature of the sol–gel solution used to fabricate high‑quality ZnO thin films via the dip‑coating method for highly sensitive UV photodetectors. Journal of the Korean Physical Society, 78, 504-509.

Kumar, H., Sharma, R., Yadav, A., and Kumari, R. (2020). Synthesis, characterization and influence of reduced Graphene Oxide (rGO) on the performance of mixed metal oxide nano-composite as optoelectronic material and corrosion inhibitor. Chemical Data Collections, 29, 100527.

Lee, K.S., Park, C.W., and Kim, J.-D. (2018). Synthesis of ZnO/active carbon with high surface area for supercapacitor electrodes. Colloids and Surfaces A, 555, 482-490.

Li, Z., Zhou, Z., Yun, G., Shi, K., Lv, X., and Yang, B. (2013). High-performance solid-state supercapacitors based on graphene-ZnO hybrid nanocomposites. Nanoscale Research Letters, 8, 473.

Lo, A.-Y., Saravanan, L., Tseng, C.-M., Wang, F.-K., and Huang, J.-T. (2020). Effect of composition ratios on the performance of graphene/carbon nanotube/manganese oxide composites toward supercapacitor applications. ACS Omega, 5, 578-587.

Lohar, G.M., Pore, O.C., and Fulari, A.V. (2021). Electrochemical behavior of CuO/rGO nanopellets for flexible supercapacitor, non-enzymatic glucose, and H2O2 sensing application. Ceramic International, 47, 16674-16687.

Luo, Q., Xu, P., Qiu, Y., Cheng, Z., Chang, X., and Fan, H. (2017). Synthesis of ZnO tetratpods for high-performance supercaapcitor applications. Materials Letters, 198, 192-195.

Maher, M., Hassan, S., Shoueir, K., Yousif, B., Eldin, M., and Elsoud, A. (2021). Activated carbon electrode with promising specific capacitance based on potassium bromide redox additive electrolyte for supercapasitor application. Journal Materials Research And Technology, 11, 1232-1244.

Maity, C. K., Hatui, G., Verma, K., Udayabhanu, G., Pathak, D.D., and Nayak, G. C. (2018). Single pot fabrication of N doped reduced GO (N-rGO)/ZnO-CuO nanocomposite as an efficient electrodematerial for supercapacitor application. Vacuum, 157, 145-154.

Majeed, A., Ullah, W., Anwar, A.W., Nasreen, F., Sharif, A., Mustafa, G., and Khan, A. (2016). Graphene-metal oxide/hydroxide nanocomposite materials: Fabrication advancements and supercapacitive performance. Journal of Alloys and Compounds, 671, 1-10.

Miah, M., Mondal, T.K., Ghosh, A., and Saha, S.K. (2020). Study of highly porous ZnO nanospheres embedded reduced graphene oxide for high performance supercapacitor application. Electrochimica Acta, 354, 136675.

Nandiyanto, A. B. D., Oktiani, R., and Ragadhita, R. (2019). How to read and interpret FTIR spectroscope of organic material. Indonesian Journal of Science and Technology, 4(1), 97-118.

Otun, K.O., Xaba, M.S., Zong, S., Liu, X., Hildebrandt, D., El-Bahy, S.M., Alotaibi, M.T., El- and Bahy, Z.M. (2022). ZIF-8-derived ZnO/C decorated hydroxyl-functionalized multi-walled carbon nanotube as a new composite electrode for supercapacitor application. Colloid and Interface Science Communiations, 47, 100589.

Park, S., An, J., Potts, J. R., Velamakanni, A., Murali, S., and Ruoff, R. S. (2011). Hydrazine-reduction of graphite-and graphene oxide. Carbon, 49, 3019-3023.

Prabhuraj, T., Prabhu, S., Dhandapani, E., Duraisamy, N., Ramesh, R., Ramesh Kumar, K.A., and Maadeswaran, P. (2021). Bifunctional ZnO sphere/r-GO composites for supercapacitor and photocatalytic activity of organic dye degradation. Diamond and Related Materials, 120, 108592.

Qin, Z., Li, Z.J., Yun, G.Q., Shi, K., Li, K., and Yang, B.C. (2014). ZnO nanorods inserted graphene sheets with improved supercapacitive performance. Applied Surface Science, 292, 544-550.

Rai, S., Bhujel, R., Khadka, M., Chetry, R.L., Swain, B.P., and Biswas, J. (2021). Synthesis, characterizations, and electrochemical studies of ZnO/reduced graphene oxide nanohybrids for supercapacitor application. Materials Today Chemistry, 20, 100472.

Ramachandran, R., Saranya, M., Kollu, P., Raghupathy, B.P.C., Jeong, S.K., and Grace, A.N. (2015). Solvothermal synthesis of Zinc sulfide decorated Graphene (ZnS/G) nanocomposites for novel supercapacitor electrodes. Electrochimica Acta, 178, 647-657.

Rao, M.P., Wu, J.J., Asiri, A.M., Anandan, S., and Ashokkumar, M. (2018). Photocatalytic propeties of hierarchical CuO nanosheet synthesized by a solution phase method. Journal of Environmental Sciences, 69, 115-124.

Sagadevan, S., Chowdhury, Z.Z., Johan, M.R.B., Aziz, F.A., Salleh, E.M., Hawa, A., and Rafique, R.F. (2018). A one-step facile route synthesis of copper oxide/reduced graphene oxide nanocomposite for supercapacitor applications. Journal of Experimental Nanoscience, 13, 284-295.

Sahu, K., and Kar, A.K. (2019). Morphological, optical, photocatalytic and electrochemical properties of hydrothermally grown ZnO nanoflowers with variation in hydrothermal temperature. Materials Science in Semiconductor Processing, 104, 104648.

Saranya, M., Ramachandran, R., and Wang, F. (2016). Graphene-zinc oxide (G-ZnO) nanocomposite for electrochemical supercapacitor applications. Journal of Science: Advanced Materials and Devices, 1, 454-460.

Selvakumar, M., Bhat, D.K., Aggarwal, A.M., Iyer, S.P., and Sravani, G. (2010). Nano ZnO-activated carbon composite electrodes for supercapacitors. Physica B, 405, 2286-2289.

Sethi, M., Shenoy, U.S., and Bhat, D.K. (2020). A porous graphene–NiFe2O4 nanocomposite with high electrochemical performance and high cycling stability for energy storage applications. Nanoscale Advances, 2, 4229-4241.

Sheikhzadeh, M., Sanjabi, S., Gorji, M., and Khabazian, S. (2018). Nano composite foam layer of CuO/graphene oxide (GO) for high performance supercapacitor. Synthetic Metals, 244, 10-14.

Soltani, T., and Lee, B.K. (2017). A benign ultrasonic route to reduced graphene oxide from pristine graphite. Journal of Colloid and Interface Science, 486, 337-343.

Tian, Z., Bai, S., Cao, K., and Li, J. (2016). Facile preparation of ZnO nanorods/reduced graphene oxide nanocomposites with photocatalytic property. Materials Express, 6, 437-443.

Wang, H., Tian, H., Wang, X., Qiao, L., Wang, S., Wang, X., Zheng, W., and Liu, Y. (2011). Electrical conductivity of alkaline-reduced graphene oxide. Chemical Research Chinese Universities, 27(5), 857-861.

Wei, G., Yan, L., Huang, H., Yan, F., Liang, X., Xu, S., Lan, Z., Zhou, W., Guo, J. (2021) The hetero-structured nanoarray construction of Co3O4 nanowires anchored on nanoflakes as a high-performance electrode for supercapacitors. Applied Surface Science, 538, 147932.

Wu, F., Wang, X., Hu, S., Hao, C., Gao, H., and Zhou, S. (2017). Solid-state preparation of CuO/ZnO nanocomposites for functional supercapacitor electrodes and photocatalysts with enhanced photocatalytic properties. International Journal of Hydrogen Energy, 42, 30098-30108.

Xie L.-J., Wu J.-F., Chen C.-M., Zhang C.-M., Wan L., Wang J.-L., Kong, Q.-Q., Lv, C.-X., Li, K.-X., and Sun, G.-H. (2013). A novel asymmetric supercapacitor with an activated carbon cathode and a reduced graphene oxide–cobalt oxide nanocomposite anode. Journal of Power Sources, 242, 148-156.

Yahia, S. B., Znaidi, L., Kanaev, A., and Petitet, J.P. (2008). Raman study of oriented ZnO thin films deposited by sol-gel method. Spectrochimica Acta Part A, 71, 1234-1238.

Zhou X. and Ma, L. (2015). MnO2/ZnO porous film: Electrochemical synthesis and enhanced supercapacitor performances. Thin Solid Films, 597, 44-49.



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