Microwave-Assisted Chemical Co-reduction of Pd Nanoparticles Anchored on Reduced Graphene Oxide with Different Loading Amounts


Dyah Ayu Fatmawati(1), Triyono Triyono(2*), Wega Trisunaryanti(3), Uswatul Chasanah(4)

(1) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(2) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(3) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(4) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(*) Corresponding Author


Microwave-assisted Palladium/Reduced Graphene Oxide (Pd/RGO) synthesis was effectively carried out in this study, which looked at the effects of different Pd loading weights in Graphene Oxide (GO) on its physicochemical qualities. The Tour technique was used to make GO, with a KMnO4:graphite weight ratio of 3.5. Meanwhile, Pd/RGO was synthesized utilizing the in-situ reduction method of one-pot synthesis with ascorbic acid as the green reducing agent, yielding Pd-0.5/RGO, Pd-1.0/RGO, and Pd-2.0/RGO, respectively, with variations in Pd loading weight of 0.5, 1.0, and 2.0%. XRD, FTIR, SAA, SEM-EDX, and TEM were used to examine all material characterizations. As a result, Pd-1.0/RGO had the largest surface area of 65.168 m2/g among the Pd-based materials, with a pore volume of 0.111 cc/g, the pore diameter of 3.316 nm, Pd crystallite size of 28.29 nm, RGO nanostructure dimension of 3.37 × 28.53 nm, and reduction level (C/O) of 3.02. This material also contains specific functional groups, including O-H, C-H, CO2, C=C, C=O, and C-O, based on FTIR spectra. Therefore, optimal weight loading of metal on the surface of the supporting material will provide a large material surface area. Increasing the surface area of the material improves its performance as a catalyst.


in-situ reduction; palladium; reduced graphene oxide; microwave, Tour method

Full Text:

Full Text PDF


[1] Dideikin, A.T., and Vul’, A.Y., 2019, Graphene oxide and derivatives: The place in graphene family, Front. Phys., 6, 149.

[2] Paulchamy, B., Arthi, G,. and Lignesh, B.D., 2015, A simple approach to stepwise synthesis of graphene oxide nanomaterial, J. Nanomed. Nanotechnol., 6 (1), 253.

[3] Alam, S.N., Sharma, N., and Kumar, L., 2017, Synthesis of graphene oxide (GO) by modified hummers method and its thermal reduction to obtain reduced graphene oxide (rGO), Graphene, 6 (1), 1–8.

[4] Kuilla, T., Bhadra, S., Yao, D., Kim, N.H., Bose, S., and Lee, J.H., 2010, Recent advances in graphene based polymer composites, Prog. Polym. Sci., 35 (11), 1350–1375.

[5] Smith, A.T., LaChance, A.M., Zeng, S., Liu, B., and Sun, L., 2019, Synthesis, properties, and applications of graphene oxide/reduced graphene oxide and their nanocomposites, Nano Mater. Sci., 1 (1), 31–47.

[6] Ranjan, P., Agrawal, S., Sinha, A., Rao, T.R., Balakrishnan, J., and Thakur, A.D., 2018, A low-cost non-explosive synthesis of graphene oxide for scalable applications, Sci. Rep., 8 (1), 12007.

[7] Benzait, Z., Chen, P., and Trabzon, L., 2021, Enhanced synthesis method of graphene oxide, Nanoscale Adv., 3 (1), 223–230.

[8] Marcano, D.C., Kosynkin, D.V., Berlin, J.M., Sinitskii, A., Sun, Z., Slesarev, A., Alemany, L.B., Lu, W., and Tour, J.M., 2010, Improved synthesis of graphene oxide, ACS Nano, 4 (8), 4806–4814.

[9] Loryuenyong, V., Totepvimarn, K., Eimburanapravat, P., Boonchompoo, W., and Buasri, A., 2013, Preparation and characterization of reduced graphene oxide sheets via water-based exfoliation and reduction methods, Adv. Mater. Sci. Eng., 2013, 923403.

[10] Abdolhosseinzadeh, S., Asgharzadeh, H., and Kim, H.S., 2015, Fast and fully-scalable synthesis of reduced graphene oxide, Sci. Rep., 5 (1), 10160.

[11] Habte, A.T., and Ayele, D.W., 2019, Synthesis and characterization of reduced graphene oxide (rGO) started from graphene oxide (GO) using the Tour method with different parameters, Adv. Mater. Sci. Eng., 2019, 5058163.

[12] Xie, X., Zhou, Y., and Huang, K., 2019, Advances in microwave-assisted production of reduced graphene oxide, Front. Chem., 7, 355.

[13] Schwenke, A.M., Hoeppener, S., and Schubert, U.S., 2015, Synthesis and modification of carbon nanomaterials utilizing microwave heating, Adv. Mater., 27 (28), 4113–4141.

[14] Mallikarjuna, K., Reddy, L.V., Al-Rasheed, S., Mohammed, A., Gedi, S., and Kim, W.K., 2021, Green synthesis of reduced graphene oxide-supported palladium nanoparticles by Coleus amboinicus and its enhanced catalytic efficiency and antibacterial activity, Crystals, 11 (2), 134.

[15] Galvan, V., Glass, D.E., Baxter, A.F., and Prakash, G.K.S., 2019, Reduced graphene oxide supported palladium nanoparticles for enhanced electrocatalytic activity toward formate electrooxidation in an alkaline medium, ACS Appl. Energy Mater., 2 (10), 7104–7111.

[16] Çetinkaya, Y., Metin, Ö., and Balci, M., 2016, Reduced graphene oxide supported nickel-palladium alloy nanoparticles as a superior catalyst for the hydrogenation of alkenes and alkynes under ambient conditions, RSC Adv., 6 (34), 28538–28542.

[17] Anasdass, J.R., Kannaiyan, P., Raghavachary, R., Gopinath, S.C.B., and Chen, Y., 2018, Palladium nanoparticle-decorated reduced graphene oxide sheets synthesized using Ficus carica fruit extract: A catalyst for Suzuki cross-coupling reactions, PLoS One, 13 (2), e0193281.

[18] Wang, B., Yan, T., Chang, T., Wei, J., Zhou, Q., Yang, S., and Fang, T., 2017, Palladium supported on reduced graphene oxide as a high-performance catalyst for the dehydrogenation of dodecahydro-N-ethylcarbazole, Carbon, 122, 9–18.

[19] Kumar, R., da Silva, E.T.S.G., Singh, R.K., Savu, R., Alaferdov, A.V., Fonseca, L.C., Carossi, L.C., Singh, A., Khandka, S., Kar, K.K., Alves, O.L., Kubota, L.T., and Moshkalev, S.A., 2018, Microwave-assisted synthesis of palladium nanoparticles intercalated nitrogen doped reduced graphene oxide and their electrocatalytic activity for direct-ethanol fuel cells, J. Colloid Interface Sci., 515, 160–171.

[20] Ng, J.C., Tan, C.Y., Ong, B.H., Matsuda, A., Basirun, W.J., Tan, W.K., Singh, R., and Yap, B.K., 2019, Nucleation and growth controlled reduced graphene oxide–supported palladium electrocatalysts for methanol oxidation reaction, Nanomater. Nanotechnol., 9, 1847980419827171.

[21] Li, M., Liu, R., Han, G., Tian, Y., Chang, Y., and Xiao, Y., 2017, Facile synthesis of Pd-Ni nanoparticles on reduced graphene oxide under microwave irradiation for formic acid oxidation, Chin. J. Chem., 35 (9), 1405–1410.

[22] Fatmawati, D.A., Triyono, T., Trisunaryanti, W., and Oktaviano, H.S., and Chasanah, U., 2021, The study of partially and fully oxidized ggraphene oxide prepared by green synthesis for wide-scale fabrication, Rasayan J. Chem., 14, 2129–2135.

[23] Chasanah, U., Trisunaryanti, W., Triyono, T., Oktaviano, H.S., and Fatmawati, D.A., 2021, The performance of green synthesis of graphene oxide prepared by modified hummers method with oxidation time variation, Rasayan J. Chem., 14 (3), 2017–2023.

[24] Fatmawati, D.A., Triyono, T., Trisunaryanti, W., Oktaviano, H.S., and Chasanah, U., 2021, The influence of permanganate enhancement to graphite on chemical structure and properties of graphene oxide material generated by improved Tour method, Indones. J. Chem., 21 (5), 1086–1096.

[25] Shao, G., Lu, Y., Wu, F., Yang, C., Zeng, F., and Wu, Q., 2012, Graphene oxide: The mechanisms of oxidation and exfoliation, J. Mater. Sci., 47 (10), 4400–4409.

[26] Bera, M., Chandravati, C., Gupta, P., and Maji, P.K., 2018, Facile one-pot synthesis of graphene oxide by sonication assisted mechanochemical approach and its surface chemistry, J. Nanosci. Nanotechnol., 18 (2), 902–912.

[27] Prabakaran, K., Jandas, P.J., Mohanty, S., and Nayak, S.K., 2018, Synthesis, characterization of reduced graphene oxide nanosheets and its reinforcement effect on polymer electrolyte for dye sensitized solar cell applications, Sol. Energy, 170, 442–453.

[28] Khan, M., Al-Marri, A.H., Khan, M., Mohri, N., Adil, S.F., Al-Warthan, A., Siddiqui, M.R.H., Alkhathlan, H.Z., Berger, R., Tremel, W., and Tahir, M.N., 2014, Pulicaria glutinosa plant extract: A green and eco-friendly reducing agent for the preparation of highly reduced graphene oxide, RSC Adv., 4 (46), 24119–24125.

[29] Zhang, J., Feng, A., Bai, J., Tan, Z., Shao, W., Yang, Y., Hong, W., and Xiao, Z., 2017, One-pot synthesis of hierarchical flower-like Pd-Cu alloy support on graphene towards ethanol oxidation, Nanoscale Res. Lett., 12 (1), 521.

[30] Stobinski, L., Lesiak, B., Malolepszy, A., Mazurkiewicz, M., Mierzwa, B., Zemek, J., Jiricek, P., and Bieloshapka, I., 2014, Graphene oxide and reduced graphene oxide studied by the XRD, TEM and electron spectroscopy methods, J. Electron. Spectrosc. Relat. Phenom., 195, 145–154.

[31] Johra, F.T., and Jung, W.G., 2015, Hydrothermally reduced graphene oxide as a supercapacitor, Appl. Surf. Sci., 357, 1911–1914.

[32] Kujur, S., and Pathak, D.D., 2020, Reduced graphene oxide-immobilized iron nanoparticles Fe(o)@rGO as heterogeneous catalyst for one-pot synthesis of series of propargylamines, Res. Chem. Intermed., 46 (1), 369–384.

[33] Thommes, M., Kaneko, K., Neimark, A.V., Olivier, J.P., Rodriguez-Reinoso, F., Rouquerol, J., and Sing, K.S.W., 2015, Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report), Pure Appl. Chem., 87 (9), 1051–1069.

[34] Grad, O., Mihet, M., Dan, M., Blanita, G., Radu, T., Berghian-Grosan, C., and Lazar, M.D., 2019, Au/reduced graphene oxide composites: Eco-friendly preparation method and catalytic applications for formic acid dehydrogenation, J. Mater. Sci., 54 (9), 6991–7004.

[35] Shruthi, T.K., Kumar, M.S., Arjunan, M., Pratap, A., and Chandrasekaran, N., 2015, Graphene oxide aided structural tailoring of 3-D N-doped amorphous carbon network for enhanced energy storage, RSC Adv., 5 (113), 93423–93432.

[36] Singh, S.B., and De, M., 2021, Improved hydrogen uptake of metal modified reduced and exfoliated graphene oxide, J. Mater. Res., 36 (15), 3109–3120.

[37] Ruiz-Garcia, C., Lei, Y., Heras, F., Elías, A.L., Terrones, M., and Gilarranz, M.A., 2019, Functional Pd/reduced graphene oxide nanocomposites: effect of reduction degree and doping in hydrodechlorination catalytic activity, J. Nanopart. Res., 21 (12), 276.

[38] Wei, L., and Mao, Y., 2016, Enhanced hydrogen storage performance of reduced graphene oxide hybrids with nickel or its metallic mixtures based on spillover mechanism, Int. J. Hydrogen Energy, 41 (27), 11692–11699.

[39] Wanderley, K.A., Leite, A.M., Cardoso, G., Medeiros, A.M., Matos, C.L., Dutra, R.C., and Suarez, P.A.Z., 2019, Graphene oxide and a GO/ZnO nanocomposite as catalysts for epoxy ring-opening of epoxidized soybean fatty acids methyl esters, Braz. J. Chem. Eng., 36 (3), 1165–1173.

[40] Azizighannad, S., and Mitra, S., 2018, Stepwise reduction of graphene oxide (GO) and its effects on chemical and colloidal properties, Sci. Rep., 8 (1), 10083.

[41] Oh, W.C., and Zhang, F.J., 2011, Preparation and characterization of graphene oxide reduced from a mild chemical method, Asian J. Chem., 23 (2), 875–879.

[42] Bugárová, N., Špitálsky, Z., Mičušík, M., Bodík, M., Šiffalovič, P., Koneracká, M., Závišová, V., Kubovčíková, M., Kajanová, I., Zaťovičová, M., Pastoreková, S., Šlouf, M., Majková, E., and Omastová, M., 2019, A multifunctional graphene oxide platform for targeting cancer, Cancers, 11 (6), 753.

DOI: https://doi.org/10.22146/ijc.73206

Article Metrics

Abstract views : 935 | views : 373

Copyright (c) 2022 Indonesian Journal of Chemistry

Creative Commons License
This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.


Indonesian Journal of Chemistry (ISSN 1411-9420 / 2460-1578) - Chemistry Department, Universitas Gadjah Mada, Indonesia.

Analytics View The Statistics of Indones. J. Chem.