A Novel and an Efficient 3-D High Nitrogen Doped Graphene Oxide Adsorbent for the Removal of Congo Red from Aqueous Solutions

Document Type: Original Research Paper

Authors

1 Department of Chemistry, Faculty of Sciences, University of Birjand, Birjand, Iran

2 Department of Chemistry, Faculty of Chemistry, Islamic Azad University, North Tehran Branch, Tehran, Iran

3 Center of Excellence in Electrochemistry, School of Chemistry, College of Science, University of Tehran, Tehran, Iran. Biosensor Research Center, Endocrinology and Metabolism Molecular-Cellular Sciences Institute, Tehran University of Medical Sciences, Tehran, Iran

Abstract

The current study both synthesizes and uses four compounds of graphene oxide (GO), nitrogen doped graphene oxide (ND-GO), high nitrogen doped graphene oxide (HND-GO), and three dimensional high nitrogen doped graphene oxide (3D-HND-GO) in order to remove a model anionic dye, Congo red (CR) from wastewaters. It also compares their carbon nano-structure, with regard to removal efficiency and finds out that 3D-HND-G yields higher efficiency in removal of CR, especially at lower pHs. This is due to its better dispersibility and greater surface area. Also, batch adsorption technique has been utilized and all involved parameters that affect the removal efficiency, e.g. initial pH, adsorbent dosage, initial CR concentration, and contact time are examined. The study applies Central Composite Design (CCD) to figure out their efficacies, with the results showing the following optimum conditions for removal of 100 ppm of CR: 4 mg/mL of the adsorbent, pH = 3, and 25 min of contact time. Furthermore, it studies the adsorption activity of the synthesized adsorbent, including kinetics, isotherm, and desorption comprehensibly. The adsorption isotherm is well-fitted through the Langmuir model, exhibiting high CR adsorption capacity. Also, CR adsorption kinetics shows that it has obeyed a pseudo-second-order kinetic model, indicating that adsorption has made the rate-limiting step. In addition, the proposed adsorbent has successfully been applied to reduce the concentration of CR as hazardous dye materials in the water and wastewater samples.

Keywords


Bouazizi, A., Breida, M., Achiou, B., Ouammou, M., Calvo, J. I., Aaddane, A. and Younssi, S. A. (2017). Removal of dyes by a new nano–TiO2 ultrafiltration membrane deposited on low-cost support prepared from natural Moroccan bentonite. Appl. Clay Sci. 149: 127-135.
Crini, G. (2006). Non-conventional low-cost adsorbents for dye removal: a review. Bioresour. Technol. 97(9), 1061-1085.
Deming, S. N. and Morgan, S. L. (1993). Experimental design: a chemometric approach. Elsevier.
Deng, D., Pan, X., Yu, L., Cui, Y., Jiang, Y., Qi, J., Li, W. X., Fu, Q., Ma, X. and Xue, Q. (2011). Toward N-doped graphene via solvothermal synthesis. Chem. Mater. 23(5); 1188-1193.
Fu, X., Bei, F., Wang, X., O'Brien, S. and Lombardi, J. R. (2010). Excitation profile of surface-enhanced Raman scattering in graphene–metal nanoparticle based derivatives. Nanoscale 2(8): 1461-1466.
Gong, K., Du, F., Xia, Z., Durstock, M. and Dai, L. (2009). Nitrogen-doped carbon nanotube arrays with high electrocatalytic activity for oxygen reduction. Sci. 323(5915): 760-764.
Hu, S., Wang, A., Li, X. and Löwe, H. (2010). Hydrothermal synthesis of well-dispersed ultrafine N-doped TiO2 nanoparticles with enhanced photocatalytic activity under visible light. J. Phys. Chem. Solids 71(3): 156-162.
Jorio, A., Dresselhaus, M., Saito, R. and Dresselhaus, G. (2011). Raman Spectroscopy in Graphene Related Systems, Swiley. VCH, Weinheim.
Khurana, I., Saxena, A., Khurana, J. M. and Rai, P. K. (2017). Removal of Dyes Using Graphene-Based Composites: a Review. Water Air Soil Pollut. 228(5): 180-197.
Konicki, W., Hełminiak, A., Arabczyk, W. and Mijowska, E. (2017). Removal of anionic dyes using magnetic Fe@ graphite core-shell nanocomposite as an adsorbent from aqueous solutions. J. Coll. Interf. Sci. 497: 155-164.
Körbahti, B. K., Artut, K., Geçgel, C. and Özer, A. (2011). Electrochemical decolorization of textile
Zeraatkar Moghaddam, A., et al.
Pollution is licensed under a "Creative Commons Attribution 4.0 International (CC-BY 4.0)"
514
dyes and removal of metal ions from textile dye and metal ion binary mixtures. Chem. Eng. J. 173(3): 677-688.
Lee, S. U., Belosludov, R. V., Mizuseki, H. and Kawazoe, Y. (2009). Designing Nanogadgetry for Nanoelectronic Devices with Nitrogen‐Doped Capped Carbon Nanotubes. Small 5(15): 1769-1775.
Liu, C. H., Wu, J. S., Chiu, H. C., Suen, S. Y. and Chu, K. H. (2007). Removal of anionic reactive dyes from water using anion exchange membranes as adsorbers. Water Res. 41(7): 1491-1500.
Liu, C., You, Y., Zhao, R., Sun, D., Zhang, P., Jiang, J., Zhu, A. and Liu, W. (2017). Biosurfactant production from Pseudomonas taiwanensis L1011 and its application in accelerating the chemical and biological decolorization of azo dyes. Ecotox. Environ. Safe. 145: 8-15.
Long, D., Li, W., Ling, L., Miyawaki, J., Mochida, I. and Yoon, S. H. (2010). Preparation of nitrogen-doped graphene sheets by a combined chemical and hydrothermal reduction of graphene oxide. Langmuir 26(20): 16096-16102.
Mittal, A., Mittal, J., Malviya, A. and Gupta, V. (2009). Adsorptive removal of hazardous anionic dye ―Congo red‖ from wastewater using waste materials and recovery by desorption. J. Coll. Interf. Sci. 340(1): 16-26.
Montgomery, D. C. (2017). Design and analysis of experiments. John Wiley & Sons.
Movahed, S.K., Dabiri, M. and Bazgir, A. (2014). Palladium nanoparticle decorated high nitrogen-doped graphene with high catalytic activity for Suzuki–Miyaura and Ullmann-type coupling reactions in aqueous media. Appl. Catal. A 488: 265-274.
O‘Neill, C., Hawkes, F. R., Hawkes, D. L., Lourenço, N. D., Pinheiro, H. M. and Delée, W. (1999). Colour in textile effluents–sources, measurement, discharge consents and simulation: a review. J. Chem. Technol. Biotechnol. 74(11): 1009-1018.
Pokhrel, D. and Viraraghavan, T. (2004). Treatment of pulp and paper mill wastewater—a review. Sci. Total Environ. 333(1): 37-58.
Repo, E., Warchoł, J. K., Bhatnagar, A., Mudhoo, A. and Sillanpää, M. (2013). Aminopolycarboxylic acid functionalized adsorbents for heavy metals removal from water. Water Res. 47(14): 4812-4832.
Robinson, T., McMullan, G., Marchant, R. and Nigam, P. (2001). Remediation of dyes in textile effluent: a critical review on current treatment technologies with a proposed alternative. Bioresour. Technol. 77(3): 247-255.
Sun, L., Wang, L., Tian, C., Tan, T., Xie, Y., Shi, K., Li, M. and Fu, H. (2012). Nitrogen-doped graphene with high nitrogen level via a one-step hydrothermal reaction of graphene oxide with urea for superior capacitive energy storage. RSC Adv. 2(10): 4498-4506.
Vijaykumar, M., Vaishampayan, P.A., Shouche, Y.S. and Karegoudar, T. (2007). Decolourization of naphthalene-containing sulfonated azo dyes by Kerstersia sp. strain VKY1. Enzyme Microb. Technol. 40(2): 204-211.
Wang, J., Shi, Z., Fan, J., Ge, Y., Yin, J. and Hu, G. (2012). Self-assembly of graphene into three-dimensional structures promoted by natural phenolic acids. J. Mater. Chem. 22(42): 22459-22466.
Wang, Q., Gao, D., Gao, C., Wei, Q., Cai, Y., Xu, J., Liu, X. and Xu, Y. (2012). Removal of a Cationic Dye by Adsorption/Photodegradation Using Electrospun PAN/O-MMT Composite Nanofibrous Membranes Coated with TiO2. Int. J. Photoenergy 2012: 680419–680426.
Weber, W. and Morris, J. (1962). Removal of biologically-resistant pollutants from waste waters by adsorption. Advances in water pollution research. 2: 231-266.
Wu, P., Qian, Y., Du, P., Zhang, H. and Cai, C. (2012). Facile synthesis of nitrogen-doped graphene for measuring the releasing process of hydrogen peroxide from living cells. J. Mater. Chem. 22(13): 6402-6412.
Yang, Z. Y., Zhang, Y. X., Jing, L., Zhao, Y. F., Yan, Y. M. and Sun, K. N. (2014). Beanpod-shaped Fe–C–N composite as promising ORR catalyst for fuel cells operated in neutral media. J. Mater. Chem. A 2(8): 2623-2627.
Zahrim, A., Tizaoui, C. and Hilal, N. (2011). Coagulation with polymers for nanofiltration pre-treatment of highly concentrated dyes: a review. Desalination 266(1): 1-16.