Synthesis of Graphite/NiO/G-OH (Nickel Oxide/Hydroxyl-Functionalized Graphene) Nanocomposite Electrode for the Electro-degradation of Remazol Black 5 (RB5) Dye
DOI:
https://doi.org/10.22146/ajche.25031Keywords:
Electro-degradation, Electrode, Graphite/NiO/G-OH, Remazol black 5Abstract
Hydroxyl-functionalized graphene (G–OH) is a graphene material containing hydroxyl (–OH) as its main functional group. A higher quantity of –OH group indicates a more electroactive oxide nature, which is highly beneficial for the electrochemical degradation of remazol black 5 (RB5). Graphite electrodes, commonly used as anodes for the oxidation of organic compounds, are composed of carbon; however, they exhibit low oxidation activity toward organic compounds and are susceptible to corrosion. Therefore, deposition of a NiO/G–OH electrocatalyst on the graphite surface is necessary to enhance both activity and stability. The G–OH synthesis was carried out using a combination of electrochemical exfoliation and ultrasonication. The graphite/NiO/G–OH electrodes were prepared by electrodeposition of NiO from a solution of NiSO₄·6H₂O and G–OH at pH 10. Both graphite and graphite/NiO/G–OH electrodes were characterized using FTIR and SEM–EDX analyses. The electrochemical degradation performance of graphite and graphite/NiO/G–OH electrode was evaluated for the degradation of RB5 under varying time, pH, and NaCl concentration conditions. FTIR and SEM–EDX characterization confirmed the successful deposition of NiO/G–OH on the graphite electrode. The optimum conditions for RB5 degradation using the graphite electrode were pH 4, 9 V, 0.10 M NaCl, and a reaction time of 60 minutes, resulting in a 94.05% reduction in absorbance. In comparison, the graphite/NiO/G–OH electrode achieved complete degradation (100% absorbance reduction) under the same pH and voltage conditions, using 0.05 M NaCl for 60 minutes. GC–MS analysis of the degradation products revealed the presence of cyclic, aromatic, and organic acids, indicating the effective breakdown of the dye molecules. Based on these findings, graphene-based electrodes show strong potential as efficient, environmentally friendly materials for the electrochemical degradation of organic pollutants.
References
Aggadi, S. El, Abbassi, Z. El, and Hourch, A. El, 2021. “Color Removal from Dye-Containing Aqueous Solutions by Electrooxidation.” Desalin. Water Treat., 215, 232–236. https://doi.org/10.5004/dwt.2021.26766
Ajeel, M.A., Aroua, M.K.T., and Daud, W.M.A.W., 2016. “Reactivity of Carbon Black Diamond Electrode During the Electro-oxidation of Remazol Brilliant Blue R.” RSC Adv., 6, 3690–3699. https://doi.org/10.1039/c5ra21487d
Basharat, F., Rana, U.A., Shahid, M., and Serwar, M., 2015. “Heat Treatment of Electrodeposited NiO Films for Improved Catalytic Water Oxidation.” RSC Adv., 5, 86713–86722. https://doi.org/10.1039/c5ra17041a
Bravo-Yumi, N., Espinoza-Montero, P., Picos-Benítez, A., Navarro-Mendoza, R., Brillas, E., and Peralta-Hernández, J.M., 2020. “Synthesis and Characterization of Sb2O5-Doped Ti/SnO2-IrO2 Anodes Toward Efficient Degradation Tannery Dyes by in Situ Generated Oxidizing Species.” Electrochim. Acta, 358, 136904. https://doi.org/10.1016/j.electacta.2020.136904
Brillas, E., and Martínez-Huitle, C.A., 2015. “Decontamination of Wastewaters Containing Synthetic Organic Dyes by Electrochemical Methods. An updated review.” Appl. Catal. B Environ., 166–167, 603–643. https://doi.org/10.1016/j.apcatb.2014.11.016
Chow, D., Burns, N., Boateng, E., van der Zalm, J., Kycia, S., and Chen, A., 2023. "Mechanical Exfoliation of Expanded Graphite to Graphene-Based Materials and Modification with Palladium Nanoparticles for Hydrogen Storage." Nanomaterials, 13, 2588. https://doi.org/10.3390/nano13182588
Cornejo, O.M., Murrieta, M.F., Castañeda, L.F., and Nava, J.L., 2019. “Characterization of The Reaction Environment in Flow Reactors Fitted with BDD Electrodes for Use in Electrochemical Advanced Oxidation Processes: A Critical Review.” Electrochim. Acta, 331. https://doi.org/10.1016/j.electacta.2019.135373
Dar, F.I., Moonooswamy, K.R., and Es-Souni, M., 2013. “Morphology and Property Control of NiO Nanostructures for Supercapacitor Applications.” Nanoscale Res. Lett., 8, 1–7. https://doi.org/10.1186/1556-276X-8-363
Ding, R., Li, X., Shi, W., Xu, Q., Wang, L., Jiang, H., Yang, Z., and Liu, E., 2016. “Mesoporous Ni-P Nanocatalysts for Alkaline Urea Electrooxidation.” Electrochim. Acta, 222, 455–462. https://doi.org/10.1016/j.electacta.2016.10.198
Droguett, T., Mora-Gómez, J., García-Gabaldón, M., Ortega, E., Mestre, S., Cifuentes, G., and Pérez-Herranz, V., 2020. “Electrochemical Degradation of Reactive Black 5 Using Two-Different Reactor Configuration.” Sci. Rep., 10, 1–11. https://doi.org/10.1038/s41598-020-61501-5
Feng, Z., Li, D., Wang, L., Sun, Q., Lu, P., Xing, P., and An, M., 2019. “A 3D Porous Ni-Zn/RGO Catalyst with Superaerophobic Surface for High-Performance Hydrazine Electrooxidation.” J. Alloys Compd., 788, 1240–1245. https://doi.org/10.1016/j.jallcom.2019.03.007
Gündüz, Z., and Atabey, M., 2019. “Effects of Operational Parameters on the Decolourisation of Reactive Red 195 Dye from Aqueous Solutions by Electrochemical Treatment.” Int. J. Electrochem. Sci., 14, 5868–5885. https://doi.org/10.20964/2019.06.37
Hamad, H., Bassyouni, D., El-Ashtoukhy, E.S., Amin, N., and Abd El-Latif, M., 2018. “Electrocatalytic Degradation and Minimization of Specific Energy Consumption of Synthetic Azo Dye from Wastewater by Anodic Oxidation Process with an Emphasis on Enhancing Economic Efficiency and Reaction Mechanism.” Ecotoxicol. Environ. Saf., 148, 501–512. https://doi.org/10.1016/j.ecoenv.2017.10.061
Htwe, Y.Z.N., Chow, W.S., Suda, Y., Thant, A.A., and Mariatti, M., 2019. “Effect of Electrolytes and Sonication Times on the Formation of Graphene Using an Electrochemical Exfoliation Process.” Appl. Surf. Sci., 469, 951–961. https://doi.org/10.1016/j.apsusc.2018.11.029
Jinisha, R., Gandhimathi, R., Ramesh, S.T., Nidheesh, P. V., and Velmathi, S., 2018. “Removal of Rhodamine B Dye from Aqueous Solution by Electro-Fenton Process Using Iron-doped Mesoporous Silica as a Heterogeneous Catalyst.” Chemosphere, 200, 446–454. https://doi.org/10.1016/j.chemosphere.2018.02.117
Jung, W.T., Jang, H.S., Jeon, J.W., and Kim, B.H., 2021. “Effect of Oxygen Functional Groups in Reduced Graphene Oxide-Coated Silk Electronic Textiles for Enhancement of NO2 Gas-Sensing Performance.” ACS Omega 6, 27080–27088. https://doi.org/10.1021/acsomega.1c03658
Kaur, P., Kushwaha, J.P., and Sangal, V.K., 2018. “Transformation Products and Degradation Pathway of Textile Industry Wastewater Pollutants in Electro-Fenton Process.” Chemosphere, 207, 690–698. https://doi.org/10.1016/j.chemosphere.2018.05.114
Kim, Y.G., and Jo, W.K., 2019. “Efficient Decontamination of Textile Industry Wastewater Using a Photochemically Stable n–n Type CdSe/Ag3PO4 Heterostructured Nanohybrid Containing Metallic Ag as a Mediator.” J. Hazard. Mater., 361, 64–72. https://doi.org/10.1016/j.jhazmat.2018.08.074
Kuchtová, G., Chýlková, J., Váňa, J., Vojs, M., and Dušek, L., 2020. “Electro-Oxidative Decolorization and Treatment of Model Wastewater Containing Acid Blue 80 on Boron Doped Diamond and Platinum Anodes.” J. Electroanal. Chem., 863. https://doi.org/10.1016/j.jelechem.2020.114036
Li, J., Guan, Q., Hong, J., and Chang, C.-T., 2019. “Electrochemical Oxidation of Azo Dye Wastewater Using Graphene-Based Electrode Materials.” J. Nanosci. Nanotechnol., 19, 7308–7314. https://doi.org/10.1166/jnn.2019.16656
Li, L., Yao, J., Fang, X., Huang, Y., and Mu, Y., 2017. “Electrolytic Ammonia Removal And Current Efficiency by A Vermiculite-Packed Electrochemical Reactor.” Sci. Rep., 7, 1–8. https://doi.org/10.1038/srep41030
Migliorini, F.L., Steter, J.R., Rocha, R.S., Lanza, M.R.V., Baldan, M.R., and Ferreira, N.G., 2016. “Efficiency Study and Mechanistic Aspects in The Brilliant Green Dye Degradation Using BDD/Ti Electrodes.” Diam. Relat. Mater., 65, 5–12. https://doi.org/10.1016/j.diamond.2015.12.013
Moreira, F.C., Boaventura, R.A.R., Brillas, E., and Vilar, V.J.P., 2017. “Electrochemical Advanced Oxidation Processes: A Review on Their Application to Synthetic and Real Wastewaters.” Appl. Catal. B Environ., 202, 217–261. https://doi.org/10.1016/j.apcatb.2016.08.037
Moreno-Palacios, A. V., Palma-Goyes, R.E., Vazquez-Arenas, J., and Torres-Palma, R.A., 2019. “Bench-scale Reactor for cefadroxil Oxidation and Elimination of Its Antibiotic Activity Using Electro-Generated Active Chlorine.” J. Environ. Chem. Eng., 7, 103173. https://doi.org/10.1016/j.jece.2019.103173
Nidheesh, P. V., Zhou, M., and Oturan, M.A., 2018. “An Overview on The Removal of Synthetic Dyes from Water by Electrochemical Advanced Oxidation Processes.” Chemosphere, 197, 210–227. https://doi.org/10.1016/j.chemosphere.2017.12.195
Parvez, K., Wu, Z.S., Li, R., Liu, X., Graf, R., Feng, X., and Müllen, K., 2014. “Exfoliation of Graphite Into Graphene in Aqueous Solutions of Inorganic Salts.” J. Am. Chem. Soc. 136, 6083–6091. https://doi.org/10.1021/ja5017156
Parvez, K., Yang, S., Feng, X., and Müllen, K., 2015. “Exfoliation of Graphene Via Wet Chemical Routes.” Synth. Met., 210, 123–132. https://doi.org/10.1016/j.synthmet.2015.07.014
Pereira, L.A., de Lima Almeida, D.A., Couto, A.B., and Ferreira, N.G., 2020. “Titanium Dioxide/Oxidized Carbon Fiber Electrodes Electrochemically Produced and their Influences on Brilliant Green Dye Degradation.” Mater. Res. Bull., 122, 110642. https://doi.org/10.1016/j.materresbull.2019.110642
Pieczyńska, A., Ossowski, T., Bogdanowicz, R., and Siedlecka, E., 2019. “Electrochemical Degradation of Textile Dyes in A Flow Reactor: Effect of Operating Conditions and Dyes Chemical Structure.” Int. J. Environ. Sci. Technol., 16, 929–942. https://doi.org/10.1007/s13762-018-1704-0
Ramalingam, S., 2019. “Nano SiC Reinforced Copper Nanocomposite by a Simple Electrodeposition Method.” Int. J. Eng. Adv. Technol., 9, 239–244. https://doi.org/10.35940/ijeat.a1153.1291s419
Rebelo, Q.H.F., Ferreira, C.S., Santos, P.L., Bonacin, J.A., Passos, R.R., Pocrifka, L.A., and Paula, M.M.S., 2019. “Synthesis and Characterization of A Nanocomposite NiO/SiO2 from A Sustainable Source of SiO2.” Part. Sci. Technol., 37, 907–911. https://doi.org/10.1080/02726351.2018.1455781
Rivera, M., Pazos, M., and Sanromán, M.Á., 2011. “Development of an Electrochemical Cell for The Removal of Reactive Black 5.” Desalination, 274, 39–43. https://doi.org/10.1016/j.desal.2011.01.074
Safarpour, M., and Khataee, A., 2018. Graphene-Based Materials for Water Purification. Nanoscale Materials in Water Purification. Elsevier Inc. https://doi.org/10.1016/B978-0-12-813926-4.00021-5
Samarghandi, M.R., Dargahi, A., Shabanloo, A., Nasab, H.Z., Vaziri, Y., and Ansari, A., 2020. “Electrochemical Degradation of Methylene Blue Dye Using A Graphite Doped PbO2 Anode: Optimization of Operational Parameters, Degradation Pathway and Improving The Biodegradability of Textile Wastewater.” Arab. J. Chem., 13, 6847–6864. https://doi.org/10.1016/j.arabjc.2020.06.038
Sandoval, M.A., Zúñiga-Mallea, N., Espinoza, L.C., Vidal, J., Jara-Ulloa, P., and Salazar, R., 2019. “Decolorization and Degradation of a Mixture of Industrial Azo Dyes by Anodic Oxidation Using a Ti/Ru0.3Ti0.7O2 (DSA-Cl2) Electrode.” Chemistry Select, 4, 13856–13866. https://doi.org/10.1002/slct.201903150
Särkkä, H., Bhatnagar, A., and Sillanpää, M., 2015. “Recent Developments of Electro-Oxidation in Water Treatment - A review.” J. Electroanal. Chem., 754, 46–56. https://doi.org/10.1016/j.jelechem.2015.06.016
Sharif, F., and Roberts, E.P.L., 2020. “Electrochemical Oxidation of An Organic Dye Adsorbed on Tin Oxide and Antimony Doped Tin Oxide Graphene Composites.” Catalysts, 10. https://doi.org/10.3390/catal10020263
Shestakova, M., and Sillanpää, M., 2017. “Electrode Materials Used for Electrochemical Oxidation of Organic Compounds in Wastewater.” Rev. Environ. Sci. Biotechnol., 16, 223–238. https://doi.org/10.1007/s11157-017-9426-1
Shetti, N.P., Malode, S.J., Malladi, R.S., Nargund, S.L., Shukla, S.S., and Aminabhavi, T.M., 2019. “Electrochemical Detection and Degradation of Textile Dye Congo Red At Graphene Oxide Modified Electrode.” Microchem. J., 146, 387–392. https://doi.org/10.1016/j.microc.2019.01.033
Tang, Y., He, D., Guo, Y., Qu, W., Shang, J., Zhou, L., Pan, R., and Dong, W., 2020. “Electrochemical Oxidative Degradation of X-6G Dye by Boron-Doped Diamond Anodes: Effect of Operating Parameters.” Chemosphere, 258, 127368. https://doi.org/10.1016/j.chemosphere.2020.127368
Thaneswari, S.A., and Lourduraj, A.J.C., 2017. “Facile Single Step Electrochemical Synthesis of Few Layered Graphene for energy storage Applications.” Arab. J. Chem., 18, 80–84.
Vacchi, I.A., Raya, J., Bianco, A., and Ménard-Moyon, C., 2018. “Controlled Derivatization of Hydroxyl Groups of Graphene Oxide in Mild Conditions.” 2D Mater., 5. https://doi.org/10.1088/2053-1583/aac8a9
Vasconcelos, V.M., Ponce-de-León, C., Rosiwal, S.M., and Lanza, M.R.V., 2019. “Electrochemical Degradation of Reactive Blue 19 Dye by Combining Boron-Doped Diamond and Reticulated Vitreous Carbon Electrodes.” Chem, Electro. Chem., 6, 3516–3524. https://doi.org/10.1002/celc.201900563
Wang, X.Q., Han, S.F., Zhang, Q.W., Zhang, N., and Zhao, D.D., 2018. “Photocatalytic Oxidation Degradation Mechanism Study of Methylene Blue Dye Waste Water with GR/iTO2.” MATEC Web Conf., 238. https://doi.org/10.1051/matecconf/201823803006
Wiratini, N.M., Trisunaryanti, W., Triyono, and Kuncaka, A., 2023. “Electrochemical Removal of Remazol Black 5 (RB-5) Using SiO2/NiO/Ni Nanocomposite Electrocatalyst Deposited on the Surface of Graphite Electrodes.” Evergreen, 10, 1274–1285. https://doi.org/10.5109/7151673
Xia, Y., Wang, G., Guo, L., Dai, Q., and Ma, X., 2019. “Electrochemical Oxidation Of Acid Orange 7 Azo Dye Using a PbO2 Electrode: Parameter Optimization, Reaction Mechanism and Toxicity Evaluation.” Chemosphere, 241, 125010. https://doi.org/10.1016/j.chemosphere.2019.125010
Yan, L., Lin, M., Zeng, C., Chen, Z., Zhang, S., Zhao, X., Wu, A., Wang, Y., Dai, L., Qu, J., Guo, M., and Liu, Y., 2012. “Electroactive and Biocompatible Hydroxyl- Functionalized Graphene by Ball Milling.” J. Mater. Chem., 22, 8367–8371. https://doi.org/10.1039/c2jm30961k
Yao, Y., Chen, Q., and Zhou, J., 2021. “Influence of Typical Electrolytes on Electrooxidation of Bio-Refractory Reactive Dye.” Int. J. Environ. Sci. Technol., 19, 1799–1810. https://doi.org/10.1007/s13762-021-03184-7
Yusbarina, Y., Roto, R., and Triyana, K., 2021. “Hydroxyl Functionalized Graphene As a Superior Anode Material for Electrochemical Oxidation of Methylene Blue.” Rasayan J. Chem., 14 (2), 1140–1147. https://doi.org/10.31788/rjc.2021.1426180
Zhang, J., Zhang, D., and Liu, Y., 2019. “Ni–SiO2 Nanoporous Composite as an Efficient Electrocatalyst for the Electrooxidation of Hydrogen Peroxide.” J. Mater. Sci. Mater. Electron., 30, 13895–13909. https://doi.org/10.1007/s10854-019-01707-0
Zhao, H.Z., Sun, Y., Xu, L.N., and Ni, J.R., 2010. “Removal of Acid Orange 7 in Simulated Wastewater Using a Three-Dimensional Electrode Reactor: Removal Mechanisms and Dye Degradation Pathway.” Chemosphere, 78, 46–51. https://doi.org/10.1016/j.chemosphere.2009.10.034.
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