Cover Image

Citrate-Zn/Al Layered Double Hydroxide as Adsorbent of Congo Red from Aqueous Solution

Nurlisa Hidayati, Neza Rahayu Palapa, Bakri Rio Rahayu, Risfidian Mohadi, Elfita Elfita, Aldes Lesbani


Layered double hydroxide (LDH) of Zn/Al and citrate-Zn/Al was prepared and used as an adsorbent of Congo red from aqueous solution. LDH was characterized by X-ray, FTIR, and BET analysis. Adsorption of Congo red was studied through kinetic, isotherm, and thermodynamic analyses. Zn/Al LDH has diffraction at 10.29o (003) with interlayer distance 8.59 Å and citrate-Zn/Al LDHs have anomalous diffraction at 7.57o (003) with interlayer distance 11.68 Å. The surface area of citrate-Zn/Al (40.50 m2 g-1) has higher than pristine LDH (1.97 m2 g-1). Adsorption of Congo red was conducted at pH 6 for Zn/Al LDH and at pH 8 for citrate-Zn/Al LDH. Adsorption of Congo red on both LDHs follows the pseudo-second-order kinetic model. The isotherm parameter follows the Freundlich isotherm model with maximum adsorption capacity 166.67 mg g-1 for Zn/Al and 249.99 mg g-1 for citrate-Zn/Al LDH. Adsorption of Congo red on both LDHs was classified as physical adsorption with energy 4.085-4.148 kJ mol-1

Full Text:



- M. K. Dahri, M. R. R. Kooh, L. B. L. Lim, Water remediation using a low-cost adsorbent walnut shell for removal of malachite green: equilibrium, kinetics, thermodynamics and regeneration studies, Journal of Environmental Chemical Engineering, 2019, 2, 1434-1444.

- M. R. Samarghandi, M. Zarrabi, M. N. Sepehr, R. Panahi, M. Foroghi, Removal of Acid Red 14 by Pumice Stone as a Low-cost Adsorbent: Kinetic and Equilibrium Study, Iranian Journal of Chemistry and Chemical Engineering, 2012, 31, 19-27.

- C. Shen, Y. Pan, D. Wu, Y. Liu, C. Ma, F. Li, H. Ma, Y. Zhang, A crosslinking-induced precipitation process for the simultaneous removal of poly(vinyl alcohol) and reactive dye: the importance of covalent bond forming and magnesium coagulation, Chemical Engineering Journal, 2019, 374, 904-913.

- P. J. Ong, S. W. Tay, L. Hong, Removal of water-soluble dyes by conjugated organic skeletons through drain flow-diffusion filtration, Journal of Environmental Chemical Engineering, 2018, 6, 4612-4622.

- M. Alizadeh, E. Ghahramani, M. Zarrabi, M. N. Sepehr, Efficient de-colorization of methylene blue by the electro-coagulation method: Comparison of iron and aluminum electrode, Iranian Journal of Chemistry and Chemical Engineering, 2015, 34, 39–47.

- X. L. Cao, Y. N. Yan, F. Y. Zhou, S. P. Sun, Tailoring nanofiltration membranes for effective removing dye intermediates in complex dye-wastewater, Journal of Membrane Science, 2020, 595, 117476.

- M. R. Samarghandi, M. Zarrabi, A. Amrane, M. M. Soori, M. N. Sepehr, Removal of acid black dye by pumice stone as a low-cost adsorbent: kinetic, thermodynamic and equilibrium studies, Environmental Engineering and Management Journal, 2013, 12, 2137-2147.

- Y. Yang, L. Yan, J. Li, J. Li, T. Yan, M. Sun, Z. Pei, Synergistic adsorption and photocatalytic reduction of Cr(VI) using Zn-Al-layered double hydroxide and TiO2 composite, Applied Surface Science, 2019, 492, 487-496.

- N. Parshi, D. Pan, V. Dhavle, B. Jana, S. Maity, J. Ganguly, fabrication of lightweight and reusable salicylaldehyde functionalized chitosan as an adsorbent for dye removal and its mechanism, International Journal of Biological Macromolecules, 2019, 141, 626-635.

- Y. Song, J. Y. Seo, H. Kim, K. Y. Beak, Structural control of cellulose nanofibrous composite membrane with metal-organic framework (ZIF-8) for highly selective removal of cationic dye, Carbohydrate Polymers, 2019, 222, 115018.

- T. Taher, D. Rohendi, R. Mohadi, A. Lesbani, Thermal and acid activation (TAA) of bentonite as an adsorbent for removal methylene blue: a kinetics and thermodynamic study, Chiang Mai Journal of Science, 2018, 45, 1770-1781.

- T. A. Aragaw, F. T. Angerasa, Adsorption of basic yellow dye dataset using Ethiopian kaolin as an adsorbent, Data in Brief, 2019, 26, 104504.

- H. Quaddari, A. Karim, B. Achiou, S. Saja, A. Aaddane, J. Bennazha, I. E. A. E. Hassani, M. Ouammou, A. Albizane, Now low-cost ultrafiltration membrane made from purified natural clays for direct red 80 dye removal, Journal of Environmental Chemical Engineering, 2019, 7, 103268.

- Q. Huang, M. Liu, J. Chen, Q. Wan, J. Tian, L. Huang, R. Jiang, Y. Wen, X. Zhang, Y Wei, Facile preparation of MoS2 based polymer composites via mussel inspired chemistry and their high efficiency for removal of organic dyes, 2017, 419, 35-44.

- G. V. Brião, S. L. Jahn, E. L. Foletto, G. L. Dotto, Highly efficient and reusable mesoporous zeolite synthetized from a biopolymer for cationic dyes adsorption, Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2018, 556, 43-50.

- N. R. Palapa, T. Taher, R. Mohadi, A. Lesbani, Removal of anionic direct dye using Zn/Al, Zn/Fe, and Zn/Cr layered double hydroxides toward the interlayer distance, Science and Technology Indonesia, 2019, 4, 70-76.

- L. M. Ahmed, M. S. Gasser, Adsorption study of anionic reactive dye from aqueous solution to Mg-Fe-CO3 layered double hydroxide (LDH), Applied Surface Science, 2012, 259,650-656.

- N. R. Palapa, R. Mohadi, A. Lesbani, Adsorption of direct yellow dye from aqueous solution by Ni/Al and Zn/Al layered double hydroxides, AIP Conference Proceeding, 2018, 2026, 020018.

- N. R. Palapa, T. Taher, R. Mohadi, M. Said, A. Lesbani, Synthesis of Ni/Al layered double hydroxides (LDHs) for adsorption of malachite green and direct yellow dyes from solution: kinetic and thermodynamic, AIP Conference Proceeding, 2018, 2026, 020033.

- G. Huang, L. Jiang, D. Wang, J. Chen, Z. Li, S. Ma, Intercalation of thiacalix[4]arene anion via calcined/restored reaction into LDH and efficient heavy metal capture, Journal of Molecular Liquids, 2016, 220, 346-353.

- T. Taher, Y. Irianty, R. Mohadi, M. Said, R. Andreas, A. Lesbani, Adsorption of cadmium(II) using Ca/Al layered double hydroxides intercalated with Keggin ion, Indonesian Journal of Chemistry, 2019, 19, 873-881.

- T. Taher, M. M. Christina, M. Said, N. Hidayati, Ferlinahayati, A. Lesbani, Removal of iron(II) using intercalated Ca/Al layered double hydroxides with [-SiW12O40]4-, Bulletin of Chemical Reaction Engineering and Catalysis, 2019, 14, 260-267.

- M. Szabados, G. Varga, Z. Kónya, Á. Kukovecz, S. Carlson, P. Sipos, I. Pálinkó, Ultrasonically-enhanced preparation, characterization of CaFe-layered double hydroxides with various interlayer halide, azide and oxo anions (CO32-, NO3-, ClO4-), Ultrasonic Sonochemistry, 2018, 40, 853-860.

- M. Shafigh, M. Hamidpour, G. Furrer, Zinc release from Zn-Mg-Fe(III)-LDH intercalated with nitrate, phosphate and carbonate: the effects of low molecular weight organic acids, Applied Clay Science, 2019, 170, 135-142.

- H. Chen, J. Lin, N. Zhang, L. Chen, S. Zhong, Y. Wang, W. Zhang, Q. Ling, Preparation of MgAl-EDTA-LDH based electrospun nanofiber membrane and its adsorption properties of copper(II) from wastewater, Journal of Hazardous Materials, 2018, 345, 1-9.

- R. Lafi, K. Charradi, M. A. Djebbi, A. B. H. Amara, A. Hafiane, Adsorption study of Congo red from aqueous solution to Mg-Al-layered double hydroxide, Advanced Powder Technology, 2016, 27, 232-237.

- F. Mohamed, M. R. Abukhadra, M. Shaban, removal of safranin dye from water using polypyrrole nanofiber/Zn-Fe layered double hydroxide nanocomposite (PpyNF/Zn-Fe LDH) of enhanced adsorption and photocatalytic properties, Science of the Total Environment, 2018, 640-641, 352-363.

- M. A. Ahmed, A. A. Brick, A. A. Mohamed, An efficient adsorption of indigo carmine dye from aqueous solution on mesoporous Mg/Fe layered double hydroxide nanoparticles prepared by controlled sol-gel route, Chemosphere, 2017, 174, 280-288.

- G. George, M. P. Saravanakumar, Facile synthesis of carbon-coated layered double hydroxide and its comparative characterization with Zn-Al LDH: application on crystal violet and malachite green dye adsorption-isotherm, kinetics and Box-Behnken design, Environment Science and Pollution Research, 2018, 25, 30236-30254.

- B. Bi, B. Xu, X. Liu, Heteropoly blue-intercalated layered double hydroxides for cationic dye removal from aqueous media, Applied Clay Science, 2011, 54, 242-247.

- N. R. Palapa, T. Taher, R. Mohadi, A. Lesbani, Kinetic aspect of direct violet adsorption on M2+/M3+ (M2+ = Zn, M3+ = Al, Fe, Cr) layered double hydroxide, AIP Conference Proceeding, 2019, 2194, 020079.

- B. R. Rahayu, T. Taher, P. L. Hariani, A. Lesbani, Congo red and direct yellow dye removal from aqueous solution by Zn/Cr layered double hydroxides, AIP Conference Proceeding, 2018, 2026, 020023.

- M. Oktriyanti, N. R. Palapa, R. Mohadi, A. Lesbani, Modification of Zn-Cr layered double hydroxide with Keggin ion [SiW12O40] as Cr(VI) adsorbent, Indonesian Journal of Environmental Management and Sustainability, 2019, 3, 93-99.

- H. N. Tran, C. C. Lin, S. H. Woo, H. P. Chao, Efficient removal of copper and lead by Mg/Al layered double hydroxides intercalated with organic acid anions: adsorption kinetics, isotherms, and thermodynamics, Applied Clay Science, 2018, 154, 17-27.

- M. L-Sánchez, G. N-Maléndez, G. Luna, V. S. Pérez, J. A. Rivera, G. Fetter, ZnAl layered double hydroxides impregnated with eucalyptus oil as efficient hybrid materials against multi-resistant bacteria, Applied Clay Science, 2018, 153, 61-69.

- H. N. Umh, Y. Kim, Sensitivity of nanoparticles’ stability at the point of zero charge (PZC), Journal of Industrial and Engineering Chemistry, 2014, 20, 3175-3178.

- Y. Wang, Y. Zhang, B. Zhou, C. Li, F. Gao, X. Wang, D. Liang, Y. Wei, In-situ observation of the growth behavior of ZnAl layered double hydroxide film using EQCM, Materials and Design, 2019, 180, 107952.

- M. Dinari, A. Haghighi, P. Asadi, Facile synthesis of ZnAl-EDTA layered double hydroxide/poly(vinyl alcohol) nanocomposites as an efficient adsorbent of Cd(II) ions from the aqueous solution, Applied Clay Science, 2019, 170, 21-28.

- S. Yudarkal, C. Garlisi, L. Özcan, M. Bellardita, G. Palmisano, Photocatalyst characterization techniques: adsorption isotherms and BET, SEM, FTIR, UV-Vis, photoluminescence, and electrochemical characterizations, Heterogeneous Photocatalysis, Elsevier, 2019, 87-152.

- N. R. Palapa, R. Mohadi, A. Rachmat, A. Lesbani, Adsorption Study of Malachite Green Removal from Aqueous Solution Using Cu/M3+ (M3+=Al, Cr) Layered Double Hydroxide, Mediterranean Journal of Chemistry, 2020, 10, 33-45.

- O. Rahmanian, S. Amini, M. Dinari, Preparation of zinc/iron layered double hydroxide intercalated by citrate anion for capturing Lead (II) from aqueous solution, Journal of Molecular Liquids, 2018, 256, 9-15.

- T. Taher, R. Mohadi, A. Lesbani, Effect of Ti4+/clay ratio on the properties of titanium pillared bentonite and its application for Cr(VI) removal, Rasayan Journal of Chemistry, 2018, 11, 1244-1254.

- M. N. Sepehr, S. Nasseri, M. Zarrabi. Removal of Cr (III) from tanning effluent by Aspergillus niger in airlift bioreactor, Separation and Purification Technology, 2012, 96, 256-262.

- T. Taher, R. Mohadi, D. Rohendi, A. Lesbani, Congo red removal from aqueous solution by acid-activated bentonite from Sorolangun: kinetic, equilibrium, and thermodynamic studies, Arab Journal of Basic and Applied Sciences, 2019, 26, 125-136.

- H. Hu, J. Liu, Z. Xu, L. Zhang, B. Cheng, W. Ho, Hierarchical porous Ni/Co-LDH hollow dodecahedron with excellent adsorption property for Congo red and Cr (VI) ions, Applied Surface Science, 2019, 478, 981-990.

- I. M. Ahmed, M. S. Gasser, Adsorption study of anionic reactive dye from aqueous solution to Mg–Fe–CO3 layered double hydroxide (LDH), Applied surface science, 2012, 259, 650-656.

- L. Lu, J. Li, D. H. Ng, P. Yang, P. Song, M. Zuo, Synthesis of novel hierarchically porous Fe3O4@MgAl–LDH magnetic microspheres and its superb adsorption properties of dye from water, Journal of Industrial and Engineering Chemistry, 2017, 46, 315-323.

- S. Yang, L. Wang, X. Zhang, W. Yang, G. Song, Enhanced adsorption of Congo red dye by functionalized carbon nanotube/mixed metal oxides nanocomposites derived from layered double hydroxide precursor, Chemical Engineering Journal, 2015, 275, 315-321.

- L. Deng, H. Zeng, Z. Shi, W. Zhang, J. Luo, Sodium dodecyl sulfate intercalated and acrylamide anchored layered double hydroxides: A multifunctional adsorbent for highly efficient removal of Congo red, Journal of colloid and interface science, 2018, 521, 172-182.

- Y. H. Jia, Z. H. Liu, Preparation of borate anions intercalated MgAl-LDHs microsphere and its calcinated product with superior adsorption performance for Congo red, Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2019, 575, 373-381.

- D. Bharali, R. C. Deka, Adsorptive removal of congo red from aqueous solution by sonochemically synthesized NiAl layered double hydroxide, Journal of environmental chemical engineering, 2017, 5, 2056-2067.

- J. Xu, D. Xu, B. Zhu, B. Cheng, C. Jiang, Adsorptive removal of an anionic dye Congo red by flower-like hierarchical magnesium oxide (MgO)-graphene oxide composite microspheres, Applied Surface Science, 2018, 435, 1136-1142.

- N. Hidayati, D. R. Apriliani, T. Taher, R. Mohadi, A. Lesbani, Adsorption of congo red using Mg/Fe and Ni/Fe layered double hydroxides, In Journal of Physics: Conference Series IOP Publishing, 2019, 1282, 012075.

- S. Agarwal, I. Tyagi, V. K. Gupta, S. Mashhadi, M. Ghasemi, Kinetic and thermodynamics of malachite green dye removal from aqueous phase using iron nanoparticles loaded on ash, Journal of Molecular Liquids, 2016, 223, 1340-1347.



  • There are currently no refbacks.

Copyright (c) 2020 Mediterranean Journal of Chemistry