High Reusability of NiAl LDH/Biochar Composite in the Removal Methylene Blue from Aqueous Solution


Aldes Lesbani(1*), Neza Rahayu Palapa(2), Rabelia Juladika Sayeri(3), Tarmizi Taher(4), Nurlisa Hidayati(5)

(1) Graduate School of Mathematics and Natural Sciences, Faculty of Mathematics and Natural Sciences, Universitas Sriwijaya, Jl. Palembang Prabumulih Km. 32, Ogan Ilir 30662, Indonesia
(2) Graduate School of Mathematics and Natural Sciences, Faculty of Mathematics and Natural Sciences, Universitas Sriwijaya, Jl. Palembang Prabumulih Km. 32, Ogan Ilir 30662, Indonesia
(3) Research Center of Inorganic Materials and Coordination Complexes, Faculty of Mathematics and Natural Sciences, Universitas Sriwijaya, Jl. Palembang Prabumulih Km. 32, Ogan Ilir 30662, Indonesia
(4) Department of Environmental Engineering, Institut Teknologi Sumatera, Jl. Terusan Ryacudu, Way Hui, Kecamatan Jati Agung, Lampung Selatan 35365, Indonesia
(5) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Sriwijaya, Jl. Palembang Prabumulih Km. 32, Ogan Ilir 30662, Indonesia
(*) Corresponding Author


Ni/Al layered double hydroxide was used as a starting material for composite formation with biochar as a matrix. The materials were characterized using X-ray, FTIR, nitrogen adsorption-desorption, thermal, and morphology analyses. The NiAl LDH/Biochar material is then used as an adsorbent of methylene blue from an aqueous solution. The factor that was influencing adsorption such as pH, time, methylene blue concentration, and temperature adsorption was studied systematically. The regeneration of adsorbent was performed to know the stability of NiAl LDH/Biochar under several cycle adsorption processes. The results showed that NiAl LDH/Biochar has a specific diffraction peak at 11.63° and 22.30°. NiAl LDH/Biochar has more than ten-fold surface area properties (438,942 m2/g) than biochar (50.936 m2/g), and Ni/Al layered double hydroxide (92.682 m2/g). The methylene blue adsorption on NiAl LDH/Biochar follows a pseudo-second-order kinetic adsorption model and classify as physical adsorption. The high reusability properties were found for NiAl LDH/Biochar, which was largely different from biochar and Ni/Al layered double hydroxide.


Ni/Al; layered double hydroxide; biochar; composite; methylene blue; adsorption; reusability

Full Text:

Full Text PDF


[1] Hu, H., Wageh, S., Al-Ghamdi, A.A., Yang, S., Tian, Z., Cheng, B., and Ho, W., 2020, NiFe-LDH nanosheet/carbon fiber nanocomposite with enhanced anionic dye adsorption performance, Appl. Surf. Sci., 511, 145570.

[2] Yaseen, M., Singh, M., and Ram, D., 2014, Growth, yield and economics of vetiver (Vetiveria zizanioides L. Nash) under intercropping system, Ind. Crops Prod., 61, 417–421.

[3] Tezcan Un, U., and Ates, F., 2019, Low-cost adsorbent prepared from poplar sawdust for removal of disperse orange 30 dye from aqueous solutions, Int. J. Environ. Sci. Technol., 16 (2), 899–908.

[4] Palapa, N.R., Juleanti, N., Taher, T., and Lesbani, A., 2020, Unique adsorption properties of malachite green on interlayer space of Cu-Al and Cu-Al-SiW12O40 layered double hydroxides, Bull. Chem. React. Eng. Catal., 15 (3), 653–661.

[5] Yan, H., Li, H., Yang, H., Li, A., and Cheng, R., 2013, Removal of various cationic dyes from aqueous solutions using a kind of fully biodegradable magnetic composite microsphere, Chem. Eng. J., 223, 402–411.

[6] Long, Y., Wang, Y., Zhang, D., Ju, P., and Sun, Y., 2016, Facile synthesis of BiOI in hierarchical nanostructure preparation and its photocatalytic application to organic dye removal and biocidal effect of bacteria, J. Colloid Interface Sci., 481, 47–56.

[7] Soleimani, K., Tehrani, A.D., and Adeli, M., 2018, Bioconjugated graphene oxide hydrogel as an effective adsorbent for cationic dyes removal, Ecotoxicol. Environ. Saf., 147, 34–42.

[8] Logita, H.H., Tadesse, A., and Kebede, T., 2015, Synthesis, characterization and photocatalytic activity of MnO2/Al2O3/Fe2O3 nanocomposite for degradation of malachite green, Afr. J. Pure Appl. Chem., 9 (11), 211–222.

[9] Meili, L., Lins, P.V., Zanta, C.L.P.S., Soletti, J.I., Ribeiro, L.M.O., Dornelas, C.B., Silva, T.L., and Vieira, M.G.A., 2019, MgAl-LDH/Biochar composites for methylene blue removal by adsorption, Appl. Clay Sci., 168, 11–20.

[10] Annadurai, G., Juang, R.S., and Lee, D.J., 2002, Use of cellulose-based wastes for adsorption of dyes from aqueous solutions, J. Hazard. Mater., 92 (3), 263–274.

[11] Elmoubarki, R., Mahjoubi, F.Z., Elhalil, A., Tounsadi, H., Abdennouri, M., Sadiq, M., Qourzal, S., Zouhri, A., and Barka, N., 2017, Ni/Fe and Mg/Fe layered double hydroxides and their calcined derivatives: Preparation, characterization and application on textile dyes removal, J. Mater. Res. Technol., 6 (3), 271–283.

[12] Özdemir, M., Durmuş, Ö., Şahin, Ö., and Saka, C., 2016, Removal of methylene blue, methyl violet, rhodamine B, alizarin red, and bromocresol green dyes from aqueous solutions on activated cotton stalks, Desalin. Water Treat., 57 (38), 18038–18048.

[13] Zhang, P., O’Connor, D., Wang, Y., Jiang, L., Xia, T., Wang, L., Tsang, D.C.W., Ok, Y.S., and Hou, D., 2020, A green biochar/iron oxide composite for methylene blue removal, J. Hazard. Mater., 384, 121286.

[14] Kubo, D., Tadanaga, K., Hayashi, A., and Tatsumisago, M., 2012, Hydroxide ion conduction in Ni-Al layered double hydroxide, J. Electroanal. Chem., 671, 102–105.

[15] Oktrianti, M., Palapa, N.R., Mohadi, R., and Lesbani, A., 2020, Effective removal of iron(II) from aqueous solution by adsorption using Zn/Cr layered double hydroxides intercalated with Keggin ion, J. Ecol. Eng., 21 (5), 63–71.

[16] Liao, X.J., and Chen, G.S., 2016, A hybrid hydrogel based on clay nanoplatelets and host-guest inclusion complexes, Chin. Chem. Lett., 27 (4), 583–587.

[17] González, M.A., Pavlovic, I., and Barriga, C., 2015, Cu(II), Pb(II) and Cd(II) sorption on different layered double hydroxides. A kinetic and thermodynamic study and competing factors, Chem. Eng. J., 269, 221–228.

[18] Guo, Y., Zhu, Z., Qiu, Y., and Zhao, J., 2013, Synthesis of mesoporous Cu/Mg/Fe layered double hydroxide and its adsorption performance for arsenate in aqueous solutions, J. Environ. Sci., 25 (5), 944–953.

[19] Kovanda, F., Jindová, E., Lang, K., Kubát, P., and Sedláková, Z., 2010, Preparation of layered double hydroxides intercalated with organic anions and their application in LDH/poly(butyl methacrylate) nanocomposites, Appl. Clay Sci., 48 (1-2), 260–270.

[20] Liu, Z., and Zhang, F.S., 2009, Removal of lead from water using biochars prepared from hydrothermal liquefaction of biomass, J. Hazard. Mater., 167 (1-3), 933–939.

[21] Tan, X., Liu, Y., Zeng, G., Wang, X., Hu, X., Gu, Y., and Yang, Z., 2015, Application of biochar for the removal of pollutants from aqueous solutions, Chemosphere, 125, 70–85.

[22] Ahmad, R., and Mondal, P.K., 2010, Application of modified water nut carbon as a sorbent in Congo red and Malachite green dye contaminated wastewater remediation, Sep. Sci. Technol., 45 (3), 394–403.

[23] Wan, S., Wang, S., Li, Y., and Gao, B., 2017, Functionalizing biochar with Mg–Al and Mg–Fe layered double hydroxides for removal of phosphate from aqueous solutions, J. Ind. Eng. Chem., 47, 246–253.

[24] Zhang, M., Gao, B., Yao, Y., and Inyang, M., 2013, Phosphate removal ability of biochar/MgAl-LDH ultra-fine composites prepared by liquid-phase deposition, Chemosphere, 92 (8), 1042–1047.

[25] Zubair, M., Manzar, M.S., Mu'azu, N.D., Anil, I., Blaisi, N.I., and Al-Harthi, M.A., 2020, Functionalized MgAl-layered hydroxide intercalated date-palm biochar for enhanced uptake of cationic dye: Kinetics, isotherm and thermodynamic studies, Appl. Clay Sci., 190, 105587.

[26] Lins, P.V.S., Henrique, D.C., Ide, A.H., da silva Duarte, J.L., Dotto, G.L., Yazidi, A., Sellaoui, L., Erto, A., Zanta, C.L.P.S., and Meili, L., 2020, Adsorption of a non-steroidal anti-inflammatory drug onto MgAl/LDH-activated carbon composite – Experimental investigation and statistical physics modeling, Colloids Surf., A, 586, 124217.

[27] Wang, S., Gao, B., Li, Y., Zimmerman, A.R., and Cao, X., 2016, Sorption of arsenic onto Ni/Fe layered double hydroxide (LDH)-biochar composites, RSC Adv., 6 (22), 17792–17799.

[28] Palapa, N.R., Mohadi, R., and Lesbani, A., 2018, Adsorption of direct yellow dye from aqueous solution by Ni/Al and Zn/Al layered double hydroxides, AIP Conf. Proc., 2026, 020018.

[29] Bai, Z., Hu, C., Liu, H., and Qu, J., 2019, Selective adsorption of fluoride from drinking water using NiAl-layered metal oxide film electrode, J. Colloid Interface Sci., 539, 146–151.

[30] Tao, X., Han, Y., Sun, C., Huang, L., and Xu, D., 2019, Plasma modification of NiAlCe–LDH as improved photocatalyst for organic dye wastewater degradation, Appl. Clay Sci., 172, 75–79.

[31] Xiao, F., Cheng, J., Cao, W., Yang, C., Chen, J., and Luo, Z., 2019, Removal of heavy metals from aqueous solution using chitosan-combined magnetic biochars, J. Colloid Interface Sci., 540, 579–584.

[32] Xia, Y., Yang, T., Zhu, N., Li, D., Chen, Z., Lang, Q., Liu, Z., and Jiao, W., 2019, Enhanced adsorption of Pb(II) onto modified hydrochar: Modeling and mechanism analysis, Bioresour. Technol., 288, 121593.

[33] Wang, T., Li, C., Wang, C., and Wang, H., 2018, Biochar/MnAl-LDH composites for Cu(ΙΙ) removal from aqueous solution, Colloids Surf., A, 538, 443–450.

[34] Shaji, A., and Zachariah, A.K., 2017, “Surface area analysis of nanomaterials, in Micro and Nano Technologies, Thermal and Rheological Measurement Techniques for Nanomaterials Characterization, Volume 3, Eds. Thomas, S., Thomas, R., Zachariah, A.K., and Mishra, R.K., Elsevier Inc., 197–231.

[35] Beakou, B.H., El Hassani, K., Houssaini, M.A., Belbahloul, M., Oukani, E., and Anouar, A., 2017, A novel biochar from Manihot esculenta Crantz waste: Application for the removal of malachite green from wastewater and optimization of the adsorption process, Water Sci. Technol., 76 (6), 1447–1456.

[36] Iftekhar, S., Ramasamy, D.L., Srivastava, V., Asif, M.B., and Sillanpää, M., 2018, Understanding the factors affecting the adsorption of Lanthanum using different adsorbents: A critical review, Chemosphere, 204, 413–430.

[37] Kushwaha, A.K., Gupta, N., and Chattopadhyaya, M.C., 2014, Removal of cationic methylene blue and malachite green dyes from aqueous solution by waste materials of Daucus carota, J. Saudi Chem. Soc., 18 (3), 200–207.

[38] Bulut, E., Özacar, M., and Şengil, İ.A., 2008, Adsorption of malachite green onto bentonite: Equilibrium and kinetic studies and process design, Microporous Mesoporous Mater., 115 (3), 234–246.

[39] Wang, Y., Zhang, Y., Li, S., Zhong, W., and Wei, W., 2018, Enhanced methylene blue adsorption onto activated reed-derived biochar by tannic acid, J. Mol. Liq., 268, 658–666.

[40] Peres, E.C., Slaviero, J.C., Cunha, A.M., Hosseini–Bandegharaei, A., and Dotto, G.L., 2018, Microwave synthesis of silica nanoparticles and its application for methylene blue adsorption, J. Environ. Chem. Eng., 6 (1), 649–659.

[41] Qiao, Y., Li, Q., Chi, H., Li, M., Lv, Y., Feng, S., Zhu, R., and Li, K., 2018, Methyl blue adsorption properties and bacteriostatic activities of Mg-Al layer oxides via a facile preparation method, Appl. Clay Sci., 163, 119–128.

[42] Hasan, R., Ying, W.J., Cheng, C.C., Jaafar, N.F., Jusoh, R., Jalil, A.A., and Setiabudi, H.D., 2020, Methylene blue adsorption onto cockle shells-treated banana pith: Optimization, isotherm, kinetic, and thermodynamic studies, Indones. J. Chem., 20 (2), 368–378.

[43] Aguiar, J.E., Bezerra, B.T.C., Braga, B.M., Lima, D.S., Nogueira, R.E.F.Q., de Lucena, S.M.P., and da Silva, I.J., 2013, Adsorption of anionic and cationic dyes from aqueous solution on non-calcined Mg-Al layered double hydroxide: Experimental and theoretical study, Sep. Sci. Technol., 48 (15), 2307–2316.

[44] Purnaningtyas, M.A.K., Sudiono, S., and Siswanta, D., 2020, Synthesis of activated carbon/chitosan/alginate beads powder as an adsorbent for methylene blue and methyl violet 2B dyes, Indones. J. Chem., 20 (5), 1119–1130.

[45] Rao, V.V.B., and Rao, S.R.M., 2006, Adsorption studies on treatment of textile dyeing industrial effluent by fly ash, Chem. Eng. J., 116 (1), 77–84.

[46] Hu, W., Wu, X., Jiao, F., Yang, W., and Zhou, Y., 2016, Preparation and characterization of magnetic Fe3O4@sulfonated β-cyclodextrin intercalated layered double hydroxides for methylene blue removal, Desalin. Water Treat., 57 (53), 25830–25841.

[47] Vadivelan, V., and Kumar, K.V., 2005, Equilibrium, kinetics, mechanism, and process design for the sorption of methylene blue onto rice husk, J. Colloid Interface Sci., 286 (1), 90–100.

[48] Yavuz, E., Bayramoğlu, G., Arica, M.Y., and and Senkal, B.F., 2011, Preparation of poly (acrylic acid) containing core-shell type resin for removal of basic dyes, J. Chem. Technol. Biotechnol., 86 (5), 699–705.

[49] Lesbani, A., Asri, F., Palapa, N.R., Taher, T., and Rachmat, A., 2020, Efficient removal of methylene blue by adsorption using composite based Ca/Al layered double hydroxide-biochar, Global NEST J., 22 (2), 250–257.

[50] Liu, J., Li, X., Luo, J., Duan, C., Hu, H., and Qian, G., 2014, Enhanced decolourisation of methylene blue by LDH-bacteria aggregates with bioregeneration, Chem. Eng. J., 242, 187–194.

[51] Taher, T., Mohadi, R., Rohendi, D., and Lesbani, A., 2017, Kinetic and thermodynamic adsorption studies of Congo red on bentonite, AIP Conf. Proc., 1823, 020028.

[52] Mahmoodi, N.M., Hayati, B., Arami, M., and Lan, C., 2011, Adsorption of textile dyes on Pine Cone from colored wastewater: Kinetic, equilibrium and thermodynamic studies, Desalination, 268 (1-3), 117–125.

DOI: https://doi.org/10.22146/ijc.56955

Article Metrics

Abstract views : 3781 | views : 2524

Copyright (c) 2021 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 /e-ISSN 2460-1578) - Chemistry Department, Universitas Gadjah Mada, Indonesia.

Analytics View The Statistics of Indones. J. Chem.