Mg-Al/Biochar Composite with Stable Structure for Malachite Green Adsorption from Aqueous Solutions

Arini Fousty Badri  -  Graduate School, Faculty of Mathematics and Natural Sciences, Universitas Sriwijaya, Indonesia
Patimah Mega Syah Bahar Nur Siregar  -  Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Sriwijaya, Indonesia
Neza Rahayu Palapa scopus  -  Graduate School, Faculty of Mathematics and Natural Sciences, Universitas Sriwijaya, Indonesia
Risfidian Mohadi scopus  -  Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Sriwijaya, Indonesia
Mardiyanto Mardiyanto scopus  -  Department of Pharmacy, Faculty of Mathematics and Natural Sciences, Universitas Sriwijaya, Indonesia
*Aldes Lesbani scopus  -  Research Center of Inorganic Materials and Complexes, Faculty of Mathematics and Natural Sciences, Universitas Sriwijaya, Indonesia
Received: 2 Feb 2021; Revised: 16 Mar 2021; Accepted: 17 Mar 2021; Published: 31 Mar 2021; Available online: 19 Mar 2021.
Open Access Copyright (c) 2021 by Authors, Published by BCREC Group
Creative Commons License This work is licensed under a Creative Commons Attribution-ShareAlike 4.0 International License.

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Mg-Al-layered double hydroxide (LDH) was fabricated using a coprecipitation method at pH 10. Thereafter, Mg-Al-LDH was impregnated with biochar to manufacture a Mg-Al/Biochar composite. The composite was characterized using powder X-ray diffraction (XRD), Fourier-transform infrared (FTIR) spectroscopy, N2 adsorption—desorption, thermogravimetry-differential thermal analysis (TG-DTA), and scanning electron microscopy (SEM) experiments, and was subsequently used for malachite green (MG) adsorption. MG adsorption experiments were performed in a batch system, and the effects of temperature and adsorption kinetic and isotherm parameters on the adsorption process were analyzed. The stability of Mg-Al/Biochar was evaluated using regeneration experiments over three cycles. The peaks at 11.47° (003), 22.86° (002), 34.69° (012), and 61.62° (116), in the XRD profile of Mg-Al/Biochar suggested that Mg-Al/Biochar was successfully fabricated. The surface area of Mg-Al/Biochar was up to five times larger than that of pristine Mg-Al-LDH. The adsorption of MG on Mg-Al/Biochar was dominated by interactions at the surface of the adsorbent and was classified as physical adsorption; moreover the maximum adsorption capacity ofMg-Al/Biochar was 70.922 mg/g. Furthermore, the MG removal of Mg-Al/Biochar during three successive adsorption cycles (i.e. 66.73%, 65.57%, and 65.77% for the first, second, and third adsorption cycle) did not change significantly, which indicated the stable structure of the adsorbent. Copyright © 2021 by Authors, Published by BCREC Group. This is an open access article under the CC BY-SA License (


Keywords: Malachite Green; Layered Double Hydroxide; Mg-Al; Biochar; Mg-Al/Biochar Adsorption
Funding: Universitas Sriwijaya under contract grant no. 0687/UN9/SK.BUK.KP/2020

Article Metrics:

  1. Santhi, T., Manonmani, S., Smitha, T. (2010). Removal of methyl red from aqueous solution by activated carbon prepared from the Annona squmosa seed by adsorption. Chemical Engineering Research Bulletin, 14, 11–18, doi: 10.3329/cerb.v14i1.3767
  2. Méndez, A., Fernández, F., Gascó, G. (2007). Removal of malachite green using carbon-based adsorbents. Desalination, 206, 147–153, doi: 10.1016/j.desal.2006.03.564
  3. Mahmoud, R.K., Kotp, A.A., El-Deen, A.G.A., Farghali, A., Abo El-Ela, F.I. (2020). Novel and Effective Zn-Al-GA LDH Anchored on Nanofibers for High-Performance Heavy Metal Removal and Organic Decontamination: Bioremediation Approach. Water, Air, and Soil Pollution, 231, 363, doi: 10.1007/s11270-020-04629-4
  4. Islam, M.A., Ali, I., Karim, S.M.A., Hossain Firoz, M.S., Chowdhury, A.N., Morton, D.W., Angove, M.J. (2019). Removal of dye from polluted water using novel nano manganese oxide-based materials. Journal of Water Process Engineering, 32, 100911, doi: 10.1016/j.jwpe.2019.100911
  5. Schwarzenbach, R.P., Egli, T., Hofstetter, T.B., von Gunten, U., Wehrli, B. (2010). Global Water Pollution and Human Health. Annual Review of Environment and Resources, 35, 109–136, doi: 10.1146/annurev-environ-100809-125342
  6. Haile, H.L., Abi, T., Tesfahun, K. (2015). Synthesis, characterization and photocatalytic activity of MnO2/Al2O3/Fe2O3 nanocomposite for degradation of malachite green. African Journal of Pure and Applied Chemistry, 9, 211–222, doi: 10.5897/ajpac2015.0656
  7. Zhang, P., Connor, D.O., Wang, Y., Jiang, L., Xia, T., Wang, L., Tsang, D.C.W., Sik, Y., Hou, D. (2020). A green biochar / iron oxide composite for methylene blue removal. Journal of Hazardous Materials, 384, 121286, doi: 10.1016/j.jhazmat.2019.121286
  8. Lü, Z., Hu, F., Li, H., Zhang, X., Yu, S., Liu, M., Gao, C. (2019). Composite nanofiltration membrane with asymmetric selective separation layer for enhanced separation efficiency to anionic dye aqueous solution. Journal of Hazardous Materials, 19, 436–443, doi: 10.1016/j.jhazmat.2019.01.086
  9. Youssef, N.A., Shaban, S.A., Ibrahim, F.A., Mahmoud, A.S. (2016). Degradation of methyl orange using Fenton catalytic reaction. Egyptian Journal of Petroleum, 25, 317–321 doi: 10.1016/j.ejpe.2015.07.017
  10. Vinsiah, R., Mohadi, R., Lesbani, A. (2020). Performance of Graphite for Congo Red and Direct Orange Adsorption. Indonesian Journal of Environmental Management and Sustainability. 4, 125-132, doi: 10.26554/ijems.2020.4.4.125-132
  11. Ríos-Badrán, I.M., Luzardo-Ocampo, I., García-Trejo, J.F., Santos-Cruz, J., Gutiérrez-Antonio, C. (2020). Production and characterization of fuel pellets from rice husk and wheat straw. Renewable Energy, 145, 500–507, doi: 10.1016/j.renene.2019.06.048
  12. Tang, H., Zhou, W., Zhang, L. (2012). Adsorption isotherms and kinetics studies of malachite green on chitin hydrogels. Journal of Hazardous Materials, 209–210, 218–225, doi: 10.1016/j.jhazmat.2012.01.010
  13. Arabkhani, P., Asfaram, A. (2020). Development of a novel three-dimensional magnetic polymer aerogel as an efficient adsorbent for malachite green removal. Journal of Hazardous Materials, 384, 121394, doi: 10.1016/j.jhazmat.2019.121394
  14. Vimonses, V., Lei, S., Jin, B., Chow, C.W.K., Saint, C. (2009). Kinetic study and equilibrium isotherm analysis of Congo Red adsorption by clay materials. Chemical Engineering Journal, 148, 354–364, doi: 10.1016/j.cej.2008.09.009
  15. Theresa, M., Ginting, S. (2017). Impregnation of bentonite with cellulose as adsorbent of congo red. Science and Technology Indonesia, 2, 37-44, doi: 10.26554/sti.2017.2.2.37-44
  16. Zubair, M., Manzar, M.S., Mu’azu, N.D., Anil, I., Blaisi, N.I., Al-Harthi, M.A. (2020). Functionalized MgAl-layered hydroxide intercalated date-palm biochar for Enhanced Uptake of Cationic dye: Kinetics, isotherm and thermodynamic studies. Applied Clay Science, 190, 105587, doi: 10.1016/j.clay.2020.105587
  17. Daud, M., Hai, A., Banat, F., Wazir, M.B., Habib, M., Bharath, G., Al-Harthi, M.A. (2019). A review on the recent advances, challenges and future aspect of layered double hydroxides (LDH)– Containing hybrids as promising adsorbents for dyes removal. Journal of Molecular Liquids, 288, 110989, doi: 10.1016/j.molliq.2019.110989
  18. Qu, J., Sha, L., Wu, C., Zhang, Q. (2019). Applications of mechanochemically prepared layered double hydroxides as adsorbents and catalysts: A mini-review. Nanomaterials, 9, 1–15, doi: 10.3390/nano9010080
  19. Ouassif, H., Moujahid, E.M., Lahkale, R., Sadik, R., Bouragba, F.Z., Sabbar, E., Diouri, M. (2020). Zinc-Aluminum layered double hydroxide: High efficient removal by adsorption of tartrazine dye from aqueous solution. Surfaces and Interfaces, 18, 100401, doi: 10.1016/j.surfin.2019.100401
  20. De Sá, F.P., Cunha, B.N., Nunes, L.M. (2013). Effect of pH on the adsorption of Sunset Yellow FCF food dye into a layered double hydroxide (CaAl-LDH-NO3). Chemical Engineering Journal, 215–216, 122–127, doi: 10.1016/j.cej.2012.11.024
  21. Lesbani, A., Asri, F., Palapa, N.R., Taher, T., Rachmat, A. (2020). Efficient removal of methylene blue by adsorption using composite based Ca/Al layered double hydroxide-biochar. Global NEST Journal, 22, 250–257, doi: 10.30955/gnj.003359
  22. El Gaini, L., Lakraimi, M., Sebbar, E., Meghea, A., Bakasse, M. (2009). Removal of indigo carmine dye from water to Mg-Al-CO3-calcined layered double hydroxides. Journal of Hazardous Materials, 161, 627–632, doi: 10.1016/j.jhazmat.2008.04.089
  23. Lafi, R., Charradi, K., Djebbi, M.A., Ben Haj Amara, A., Hafiane, A. (2016). Adsorption study of Congo red dye from aqueous solution to Mg-Al-layered double hydroxide. Advanced Powder Technology, 27, 232–237, doi: 10.1016/j.apt.2015.12.004
  24. Hu, H., Wageh, S., Al-Ghamdi, A.A., Yang, S., Tian, Z., Cheng, B., Ho, W. (2020). NiFe-LDH nanosheet/carbon fiber nanocomposite with enhanced anionic dye adsorption performance. Applied Surface Science, 511, 145570, doi: 10.1016/j.apsusc.2020.145570
  25. Meili, L., Lins, P.V., Zanta, C.L.P.S., Soletti, J.I., Ribeiro, L.M.O., Dornelas, C.B., Silva, T.L., Vieira, M.G.A. (2019). MgAl-LDH/Biochar composites for methylene blue removal by adsorption. Applied Clay Science, 168, 11–20, doi: 10.1016/j.clay.2018.10.012
  26. Zubair, M., Saood, M., Dalhat, N., Anil, I. (2020). Applied Clay Science Functionalized MgAl-layered hydroxide intercalated date-palm biochar for Enhanced Uptake of Cationic dye : Kinetics , isotherm and thermodynamic studies. Applied Clay Science, 190, 105587, doi: 10.1016/j.clay.2020.105587
  27. Amin, M.T., Alazba, A.A., Shafiq, M. (2020). LDH of NiZnFe and its composites with carbon nanotubes and data-palm biochar with efficient adsorption capacity for RB5 dye from aqueous solutions: Isotherm, kinetic, and thermodynamics studies. Current Applied Physics, (Article in Press), Available online 31 July 2020, doi: 10.1016/j.cap.2020.07.005
  28. Palapa, N.R., Taher, T., Rahayu, B.R., Mohadi, R., Rachmat, A., Lesbani, A. (2020). CuAl LDH/Rice Husk Biochar Composite for Enhanced Adsorptive Removal of Cationic Dye from Aqueous Solution. Bulletin of Chemical Reaction Engineering & Catalysis, 15(2), 525–537, doi: 10.9767/bcrec.15.2.7828.525-537
  29. Pang, X., Chen, L., Liu, Y., Chi, M., Li, Z., Plank, J. (2017). Growth behavior of water dispersed MgAl layered double hydroxide nanosheets. RSC Advances, 7, 14989–14997, doi: 10.1039/C7RA00833C
  30. 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.d.P.e.S., Meili, L. (2020). Adsorption of a non-steroidal anti-inflammatory drug onto MgAl/LDH-activated carbon composite – Experimental investigation and statistical physics modeling. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 586, 124217, doi: 10.1016/j.colsurfa.2019.124217
  31. Kang, D., Yu, X., Tong, S., Ge, M., Zuo, J., Cao, C., Song, W. (2013). Performance and mechanism of Mg/Fe layered double hydroxides for fluoride and arsenate removal from aqueous solution. Chemical Engineering Journal, 228, 731–740, doi: 10.1016/j.cej.2013.05.041
  32. Clark, I., Smith, J., Gomes, R.L., Lester, E. (2019). Continuous Synthesis of Zn2Al-CO3 Layered Double Hydroxides for the Adsorption of Reactive Dyes from Water. Journal of Environmental Chemical Engineering, 7, 2213-2929, doi : 10.1016/j.jece.2019.103175
  33. Modwi, A., Abbo, M.A., Hassan, E.A., Al-Duaij, O.K., Houas, A. (2017). Adsorption kinetics and photocatalytic degradation of malachite green (MG) via Cu/ZnO nanocomposites. Journal of Environmental Chemical Engineering, 5, 5954–5960, doi: 10.1016/j.jece.2017.11.024
  34. Huang, Q., Song, S., Chen, Z., Hu, B., Chen, J., Wang, X. (2019). Biochar-based materials and their applications in removal of organic contaminants from wastewater: state-of-the-art review. Biochar, 1, 45–73, doi: 10.1007/s42773-019-00006-5
  35. Khan, M.A., Alqadami, A.A., Otero, M., Siddiqui, M.R., Alothman, Z.A., Alsohaimi, I., Rafatullah, M., Hamedelniel, A.E. (2019). Heteroatom-doped magnetic hydrochar to remove post-transition and transition metals from water: Synthesis, characterization, and adsorption studies. Chemosphere, 218, 1089–1099, doi: 10.1016/j.chemosphere.2018.11.210
  36. Menya, E., Olupot, P.W., Storz, H., Lubwama, M., Kiros, Y., John, M.J. (2020). Optimization of pyrolysis conditions for char production from rice husks and its characterization as a precursor for production of activated carbon. Biomass Conversion and Biorefinery, 10, 57–72, doi: 10.1007/s13399-019-00399-0
  37. Palapa, N.R., Juleanti, N.N., Mohadi, R., Taher, T., Rachmat, A., Lesbani, A. (2020). Copper Aluminum Layered Double Hydroxide Modified by Biochar and its Application as an Adsorbent for Procion Red. Journal of Water and Environment Technology, 18, 359–371, doi: 10.2965/JWET.20-059
  38. Ahmed, D.N., Naji, L.A., Faisal, A.A.H., Al-Ansari, N., Naushad, M. (2020). Waste foundry sand/MgFe-layered double hydroxides composite material for efficient removal of Congo red dye from aqueous solution. Scientific Reports, 10, 1–12, doi: 10.1038/s41598-020-58866-y
  39. Qu, W., Yuan, T., Yin, G., Xu, S., Zhang, Q., Su, H. (2019). Effect of properties of activated carbon on malachite green adsorption. Fuel, 249, 45–53, doi: 10.1016/j.fuel.2019.03.058
  40. Lee, Y.C., Amini, M.H.M., Sulaiman, N.S., Mazlan, M., Boon, J.G. (2018). Batch adsorption and isothermic studies of malachite green dye adsorption using leucaena leucocephala biomass as potential adsorbent in water treatment. Songklanakarin Journal of Science and Technology, 40, 563–569, doi: 10.14456/sjst-psu.2018.67
  41. Segun Esan, O. (2019). The Removal of Single and Binary Basic Dyes from Synthetic Wastewater Using Bentonite Clay Adsorbent. American Journal of Polymer Science and Technology, 5, 16, doi: 10.11648/j.ajpst.20190501.13
  42. Abdel Salam, M., Abukhadra, M.R., Adlii, A. (2020). Insight into the Adsorption and Photocatalytic Behaviors of an Organo-bentonite/CO3O4 Green Nanocomposite for Malachite Green Synthetic Dye and Cr(VI) Metal Ions: Application and Mechanisms. ACS Omega, 5, 6, 2766–2778, doi: 10.1021/acsomega.9b03411
  43. Biswas, S., Sharma, S., Mukherjee, S., Meikap, B.C., Sen, T.K. (2020). Process modelling and optimization of a novel Semifluidized bed adsorption column operation for aqueous phase divalent heavy metal ions removal. Journal of Water Process Engineering, Elsevier. 37, 101406, doi: 10.1016/j.jwpe.2020.101406
  44. Rajabi, M., Mirza, B., Mahanpoor, K., Mirjalili, M., Najafi, F., Moradi, O., Sadegh, H., Shahryari-ghoshekandi, R., Asif, M., Tyagi, I., Agarwal, S., Gupta, V.K. (2016). Adsorption of malachite green from aqueous solution by carboxylate group functionalized multi-walled carbon nanotubes: Determination of equilibrium and kinetics parameters. Journal of Industrial and Engineering Chemistry, 34, 130–138, doi: 10.1016/j.jiec.2015.11.001
  45. George, G., Saravanakumar, M.P. (2018). Facile synthesis of carbon-coated layered double hydroxide and its comparative characterisation with Zn–Al LDH: application on crystal violet and malachite green dye adsorption—isotherm, kinetics and Box-Behnken design. Environmental Science and Pollution Research, 25, 30236–54, doi: 10.1007/s11356-018-3001-3
  46. Nasiri Azad, F., Ghaedi, M., Dashtian, K., Hajati, S., Goudarzi, A., Jamshidi, M. (2015). Enhanced simultaneous removal of malachite green and safranin O by ZnO nanorod-loaded activated carbon: Modeling, optimization and adsorption isotherms. New Journal of Chemistry, 39, 7998–8005, doi: 10.1039/c5nj01281c
  47. Mashkoor, F., Nasar, A. (2019). Preparation, characterization and adsorption studies of the chemically modified Luffa aegyptica peel as a potential adsorbent for the removal of malachite green from aqueous solution. Journal of Molecular Liquids, 274, 315–327, doi: 10.1016/j.molliq.2018.10.119
  48. Rangabhashiyam, S., Balasubramanian, P. (2018). Performance of novel biosorbents prepared using native and NaOH treated Peltophorum pterocarpum fruit shells for the removal of malachite green. Bioresource Technology Reports, 3, 75–81, doi: 10.1016/j.biteb.2018.06.004
  49. Lesbani, A., Taher, T., Palapa, N.R., Mohadi, R., Rachmat, A., Mardiyanto. (2020). Preparation and utilization of Keggin-type polyoxometalate intercalated Ni–Fe layered double hydroxides for enhanced adsorptive removal of cationic dye. SN Applied Sciences, 2, 4–7, doi: 10.1007/s42452-020-2300-8
  50. Amin, R.M., Taha, M., Abdel Moaty, S.A., Abo El-Ela, F.I., Nassar, H.F., Gadelhak, Y., Mahmoud, R.K. (2019). Gamma radiation as a green method to enhance the dielectric behaviour, magnetization, antibacterial activity and dye removal capacity of Co-Fe LDH nanosheets. RSC Advances, 9, 32544–92561, doi: 10.1039/c9ra06509a
  51. Palapa, N.R., Mohadi, R., Rachmat, A., Lesbani, A. (2020). Adsorption Study of Malachite Green Removal from Aqueous Solution Using Cu / M3+ ( M3+ = Al , Cr ) Layered Double Hydroxide. Mediterranean Journal of Chemistry, 10, 33–45, doi: 10.13171/mjc10102001261236al
  52. Sriram, G., Uthappa, U.T., Losic, D., Kigga, M., Jung, H.Y., Kurkuri, M.D. (2020). Mg-Al-layered double hydroxide (LDH) modified diatoms for highly efficient removal of Congo red from aqueous solution. Applied Sciences, 10(7), 2285, doi: 10.3390/app10072285

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