Abstract
This study focused on the functionalization of cellulose nanocrystals (CNC) with Mg/Fe-LDH composites to assess the performance and mechanism for tetracycline (TRC) removal from aqueous solutions. SEM images and the XRD patterns confirmed the cellulose nanocrystals have adhered over the surface of MgFe-LDH. The presence of CNCs over the LDH has considerably increased the specific surface area (107 to 158 m2/g) and the adsorption % of removal. The presence of salt ions in the solution was found to reduce the elimination of TRC (1.89–61% for NaHCO3). The adsorption was fast reaching the maximum adsorption capacity after 180 min of contact. The equilibrium data were better fitted by the Langmuir model reaching a maximum adsorption capacity of 165.49 mg/g. Thermodynamics indicated an endothermic and spontaneous adsorption. Finally, the composite appears to hold great potential in purifying water systems by effectively removing pharmaceutical compounds.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
Availability of Data and Materials
Data are available on request from the authors.
References
Abbasi, M., Sabzehmeidani, M. M., Ghaedi, M., Jannesar, R., & Shokrollahi, A. (2021). Adsorption performance of calcined copper-aluminum layered double hydroxides/CNT/PVDF composite films toward removal of carminic acid. Journal of Molecular Liquids, 329, 115558. https://doi.org/10.1016/j.molliq.2021.115558
Ahmad, T., Mansha, M., Kazi, I. W., Waheed, A., & Ullah, N. (2021). Synthesis of 3,5-diaminobenzoic acid containing crosslinked porous polyamine resin as a new adsorbent for efficient removal of cationic and anionic dyes from aqueous solutions. Journal of Water Process Engineering, 43, 102304. https://doi.org/10.1016/j.jwpe.2021.102304
Alagha, O., Manzar, M. S., Zubair, M., Anil, I., Muazu, N. D., & Qureshi, A. (2020). Magnetic Mg-Fe/LDH intercalated activated carbon composites for nitrate and phosphate removal from wastewater: Insight into behavior and mechanisms. Nanomaterials, 10(7), 1361. https://doi.org/10.3390/nano10071361
Alam, U., Fleisch, M., Kretschmer, I., Bahnemann, D., & Muneer, M. (2017). One-step hydrothermal synthesis of Bi-TiO2 nanotube/graphene composites: An efficient photocatalyst for spectacular degradation of organic pollutants under visible light irradiation. Applied Catalysis b: Environmental, 218, 758–769. https://doi.org/10.1016/j.apcatb.2017.06.016
Alam, U., Pandey, K., & Verma, N. (2022). Photocatalytic oxidation of glyphosate and reduction of Cr(VI) in water over ACF-supported CoNiWO4-GCN composite under batch and flow conditions. Chemosphere, 297, 134119. https://doi.org/10.1016/j.chemosphere.2022.134119
Allen, S. J., Mckay, G., & Porter, J. F. (2004). Adsorption isotherm models for basic dye adsorption by peat in single and binary component systems. Journal of Colloid and Interface Science, 280(2), 322–33. https://doi.org/10.1016/j.jcis.2004.08.078
Azizian, S., Haerifar, M., & Basiri-Parsa, J. (2007). Extended geometric method: A simple approach to derive adsorption rate constants of langmuir–freundlich kinetics. Chemosphere, 68(11), 2040–46. https://doi.org/10.1016/j.chemosphere.2007.02.042
Blaisi, N. I., Zubair, M., Ihsanullah, S. A., Kazeem, T. S., Manzar, M. S., Al-Kutti, W., & Al Harthi, M. A. (2018). Date palm Ash-MgAl-layered double hydroxide composite: Sustainable adsorbent for effective removal of methyl orange and eriochrome black-T from aqueous phase. Environmental Science and Pollution Research, 25(34), 34319–34331. https://doi.org/10.1007/s11356-018-3367-2
Bonilla-Petriciolet, Adrián, Mendoza-Castillo, DI, and Reynel-Ávila HE (2017) “Adsorption processes for water treatment and purification.” Adsorption Processes for Water Treatment and Purification, no. July: 1–256. https://doi.org/10.1007/978-3-319-58136-1.
Charuaud, L., Jarde, E., Jaffrezic, A., Thomas, M. F., & Le Bot, B. (2019). Veterinary pharmaceutical residues from natural water to tap water: Sales, occurrence and fate. Journal of Hazardous Materials, 361, 169–86. https://doi.org/10.1016/j.jhazmat.2018.08.075
Chen, J., Yu, X., Li, C., Tang, X., & Sun, Y. (2020). Removal of tetracycline via the synergistic effect of biochar adsorption and enhanced activation of persulfate. Chemical Engineering Journal, 382, 122916. https://doi.org/10.1016/j.cej.2019.122916
Chengqian, F., Wanbing, L., Yimin, D., Zhiheng, W., Yaqi, L., Ling, C., Bo, L., et al. (2023). Synthesis of a novel hierarchical pillared Sep@Fe3O4/ZnAl-LDH composite for effective anionic dyes removal. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 663, 130921. https://doi.org/10.1016/j.colsurfa.2023.130921
Daghrir, R., & Drogui, P. (2013). Tetracycline antibiotics in the environment: A review. Environmental Chemistry Letters, 11(3), 209–227.
Dai, Y., Zhang, K., Meng, X., Li, J., Guan, X., Sun, Q., Sun, Y., et al. (2019). New use for spent coffee ground as an adsorbent for tetracycline removal in water. Chemosphere, 215, 163–72. https://doi.org/10.1016/j.chemosphere.2018.09.150
Das, A., Jana, A., Das, D., Biswas, S., Sheshadri, H., Rao, M. S., & De, S. (2023). Surfactant assisted APTES functionalization of graphene oxide intercalated layered double hydroxide (LDH) for uranium adsorption from alkaline leach liquor. Journal of Cleaner Production, 390, 136058. https://doi.org/10.1016/j.jclepro.2023.136058
Dotto, G. L., Vieira, M. L. G., Esquerdo, V. M., & Pinto, L. A. A. (2013). Equilibrium and thermodynamics of azo dyes biosorption onto spirulina platensis. Brazilian Journal of Chemical Engineering, 30(1), 13–21. https://doi.org/10.1590/S0104-66322013000100003
El Messaoudi, N., El Khomri, M., Chegini, Z. G., Bouich, A., Dbik, A., Bentahar, S., Labjar, N., Iqbal, M., Jada, A., & Lacherai, A. (2022b). Dye removal from aqueous solution using nanocomposite synthesized from oxalic acid-modified agricultural solid waste and ZnFe2O4 nanoparticles. Nanotechnology for Environmental Engineering, 7(3), 797–811. https://doi.org/10.1007/s41204-021-00173-6
El Messaoudi, N., El Mouden, A., Fernine, Y., El Khomri, M., Bouich, A., Faska, N., Ciğeroğlu, Z., Américo-Pinheiro, J. H. P., Jada, A., & Lacherai, A. (2022d). Green synthesis of Ag2O nanoparticles using punica granatum leaf extract for sulfamethoxazole antibiotic adsorption: Characterization, experimental study, modeling, and DFT calculation. Environmental Science and Pollution Research. https://doi.org/10.1007/s11356-022-21554-7
Fan, S., Wang, Yi., Li, Y., Wang, Z., Xie, Z., & Tang, J. (2018). Removal of tetracycline from aqueous solution by biochar derived from rice straw. Environmental Science and Pollution Research, 25(29), 29529–29540. https://doi.org/10.1007/s11356-018-2976-0
GaniyuSoliu, O., van Hullebusch, E. D., Cretin, M., Esposito, G., & Oturan, M. A. (2015). Coupling of membrane filtration and advanced oxidation processes for removal of pharmaceutical residues: A critical review. Separation and Purification Technology, 156, 891–914. https://doi.org/10.1016/j.seppur.2015.09.059
Gao, M., Zhang, Y., Gong, X., Song, Z., & Guo, Z. (2018). Removal mechanism of Di-n-Butyl phthalate and oxytetracycline from aqueous solutions by nano-manganese dioxide modified biochar. Environmental Science and Pollution Research, 25(8), 7796–7807. https://doi.org/10.1007/s11356-017-1089-5
Gao, F., Xu, Z., & Dai, Y. (2021). Removal of tetracycline from wastewater using magnetic biochar: A comparative study of performance based on the preparation method. Environmental Technology & Innovation, 24, 101916. https://doi.org/10.1016/j.eti.2021.101916
Henrique, D. C., Quintela, D. U., Ide, A. H., Erto, A., da Silva Duarte, J. L., & Meili, L. (2020). Calcined mytella falcata shells as alternative adsorbent for efficient removal of rifampicin antibiotic from aqueous solutions. Journal of Environmental Chemical Engineering, 8(3), 103782. https://doi.org/10.1016/j.jece.2020.103782
Ho, Y. S., & McKay, G. (1999). Pseudo-second order model for sorption processes. Process Biochemistry, 34(5), 451–465. https://doi.org/10.1016/S0032-9592(98)00112-5
Hoslett, J., Ghazal, H., Katsou, E., & Jouhara, H. (2021). The removal of tetracycline from water using biochar produced from agricultural discarded material. Science of The Total Environment, 751, 141755. https://doi.org/10.1016/j.scitotenv.2020.141755
Hossain, M. A., Kumita, M., Michigami, Y., & Mori, S. (2005). Kinetics of Cr(VI) adsorption on used black tea leaves. Journal of Chemical Engineering of Japan, 38(6), 402–408. https://doi.org/10.1252/jcej.38.402
Huang, D., Liu, C., Zhang, C., Deng, R., Wang, R., Xue, W., Luo, H., Zeng, G., Zhang, Q., & Guo, X. (2019a). Cr(VI) removal from aqueous solution using biochar modified with Mg/Al-layered double hydroxide intercalated with ethylenediaminetetraacetic acid. Bioresource Technology, 276, 127–32. https://doi.org/10.1016/j.biortech.2018.12.114
Huang, Y., Zhao, X., Yuangang, Zu., Wang, Lu., Deng, Y., Mingfang, Wu., & Wang, H. (2019b). Enhanced solubility and bioavailability of apigenin via preparation of solid dispersions of mesoporous silica nanoparticles. Iranian Journal of Pharmaceutical Research : IJPR, 18(1), 168–182.
Ishak, W. H., Wan, I. A., Ramli, S., & Amin, M. C. I. M. (2018). Gamma irradiation-assisted synthesis of cellulose nanocrystal-reinforced gelatin hydrogels. Nanomaterials, 8(10), 1–13. https://doi.org/10.3390/nano8100749
Jain, A., Balasubramanian, R., & Srinivasan, M. P. (2016). Hydrothermal conversion of biomass waste to activated carbon with high porosity: A review. Chemical Engineering Journal, 283(January), 789–805. https://doi.org/10.1016/j.cej.2015.08.014
Javid, A., Mesdaghinia, A., Nasseri, S., Mahvi, A. H., Alimohammadi, M., & Gharibi, H. (2016). Assessment of tetracycline contamination in surface and groundwater resources proximal to animal farming houses in Tehran, Iran. Journal of Environmental Health Science and Engineering, 14(1), 1–5. https://doi.org/10.1186/s40201-016-0245-z
Khomri, M. E., Messaoudi, N. E., Dbik, A., Bentahar, S., & Lacherai, A. (2020). Efficient adsorbent derived from argania spinosa for the adsorption of cationic dye: Kinetics, mechanism, isotherm and thermodynamic study. Surfaces and Interfaces, 20, 100601. https://doi.org/10.1016/j.surfin.2020.100601
Kim, Y., Jeong, D., Park, K. H., Yu, J. H., & Jung, S. (2018). Efficient Adsorption on benzoyl and stearoyl cellulose to remove phenanthrene and pyrene from aqueous solution. Polymers, 10(9), 1042. https://doi.org/10.3390/POLYM10091042
Liu, J., Wu, P., Li, S., Chen, M., Cai, W., Zou, D., Zhu, N., & Dang, Z. (2019). Synergistic deep removal of As(III) and Cd(II) by a calcined multifunctional MgZnFe-CO3 layered double hydroxide: Photooxidation, precipitation and adsorption. Chemosphere, 225, 115–25. https://doi.org/10.1016/j.chemosphere.2019.03.009
Lu, P., & Hsieh, Y. L. (2010). Preparation and properties of cellulose nanocrystals: Rods, spheres, and network. Carbohydrate Polymers, 82(2), 329–36. https://doi.org/10.1016/j.carbpol.2010.04.073
Lyu, J., Hu, Z., Li, Z., & Ge, M. (2019). Removal of tetracycline by BiOBr microspheres with oxygen vacancies: Combination of adsorption and photocatalysis. Journal of Physics and Chemistry of Solids, 129, 61–70. https://doi.org/10.1016/j.jpcs.2018.12.041
Messaoudi, N. E., Khomri, M. E., Ablouh, E. H., Bouich, A., Lacherai, A., Jada, A., Lima, E. C., & Sher, F. (2022a). Biosynthesis of SiO2 nanoparticles using extract of nerium oleander leaves for the removal of tetracycline antibiotic. Chemosphere, 287, 132453. https://doi.org/10.1016/j.chemosphere.2021.132453
Messaoudi, N. E., Khomri, M. E., Fernine, Y., Bouich, A., Lacherai, A., Jada, A., Sher, F., & Lima, E. C. (2022b). Hydrothermally engineered eriobotrya japonica leaves/MgO nanocomposites with potential applications in wastewater treatment. Groundwater for Sustainable Development, 16, 100728. https://doi.org/10.1016/j.gsd.2022.100728
Milonjić, S. K. (2007). A consideration of the correct calculation of thermodynamic parameters of adsorption. Journal of the Serbian Chemical Society, 72(12), 1363–1367. https://doi.org/10.2298/JSC0712363M
Missau, J., Bertuol, D. A., & Tanabe, E. H. (2021). Highly efficient adsorbent for removal of crystal violet dye from aqueous solution by CaAl/LDH supported on biochar. Applied Clay Science, 214, 106297. https://doi.org/10.1016/j.clay.2021.106297
Mouden, A. E., Messaoudi, N. E., Guerraf, A. E., Bouich, A., Mehmeti, V., Lacherai, A., Jada, A., & Sher, F. (2023). Multifunctional cobalt oxide nanocomposites for efficient removal of heavy metals from aqueous solutions. Chemosphere, 317, 137922. https://doi.org/10.1016/j.chemosphere.2023.137922
Nasiruddin khan, M., & Sarwar, A. (2007). Determination of points of zero charge of natural and treated adsorbents. Surface Review and Letters, 14(03), 461–469. https://doi.org/10.1142/S0218625X07009517
Nguyen, V. T., Nguyen, T. B., Huang, C. P., Chen, C. W., Bui, X. T., & Dong, C. D. (2021). Alkaline modified biochar derived from spent coffee ground for removal of tetracycline from aqueous solutions. Journal of Water Process Engineering, 40, 101908. https://doi.org/10.1016/j.jwpe.2020.101908
Pan, J., Bai, X., Li, Y., Yang, B., Yang, P., Yu, F., & Ma, J. (2022). HKUST-1 derived carbon adsorbents for tetracycline removal with excellent adsorption performance. Environmental Research, 205, 112425. https://doi.org/10.1016/j.envres.2021.112425
Ramos-Ramírez, E., Tzompantzi-Morales, F., Gutiérrez-Ortega, N., Mojica-Calvillo, H. G., & Castillo-Rodríguez, J. (2019). Photocatalytic degradation of 246-trichlorophenol by MgO–MgFe2O4 derived from layered double hydroxide structures. Catalysts, 9(5), 454. https://doi.org/10.3390/catal9050454
Shen, Q., Wang, Z., Yu, Q., Cheng, Y., Liu, Z., Zhang, T., & Zhou, S. (2020). Removal of tetracycline from an aqueous solution using manganese dioxide modified biochar derived from chinese herbal medicine residues. Environmental Research, 183, 109195. https://doi.org/10.1016/j.envres.2020.109195
Sheng, T., Zhang, Z., Yuncheng, Hu., Tao, Y., Zhang, J., Shen, Z., Feng, J., & Zhang, A. (2019). Adsorption of phosphorus by using magnetic Mg–Al-, Zn–Al- and Mg–Fe-layered double hydroxides: Comparison studies and adsorption mechanism. Environmental Science and Pollution Research, 26(7), 7102–7114. https://doi.org/10.1007/s11356-019-04191-5
Sokol, D., Vieira, D. E. L., Zarkov, A., Ferreira, M. G. S., Beganskiene, A., Rubanik, V. V., Shilin, A. D., Kareiva, A., & Salak, A. N. (2019). Sonication accelerated formation of Mg-Al-phosphate layered double hydroxide via sol-gel prepared mixed metal oxides. Scientific Reports, 9(1), 1–9. https://doi.org/10.1038/s41598-019-46910-5
Thakur, M., Sharma, A., Ahlawat, V., Bhattacharya, M., & Goswami, S. (2020). Process optimization for the production of cellulose nanocrystals from rice straw derived α-cellulose. Materials Science for Energy Technologies, 3, 328–334. https://doi.org/10.1016/j.mset.2019.12.005
Vieira, A. P., Santana, S. A. A., Bezerra, C. W. B., Silva, H. S. A., Chaves, J. A. P., de Melo, J. C. P., da Silva Filho, E. C., & Airoldi, C. (2009). Kinetics and thermodynamics of textile dye adsorption from aqueous solutions using babassu coconut mesocarp. Journal of Hazardous Materials, 166(2), 1272–78. https://doi.org/10.1016/j.jhazmat.2008.12.043
Wang, J., & Zhuan, R. (2020). Degradation of antibiotics by advanced oxidation processes: An overview. Science of The Total Environment, 701, 135023. https://doi.org/10.1016/j.scitotenv.2019.135023
Wang, X., Zhu, X., & Meng, X. (2017a). Preparation of a Mg/Al/Fe layered supramolecular compound and application for removal of Cr(VI) from laboratory wastewater. RSC Advances, 7(56), 34984–34993. https://doi.org/10.1039/c7ra04646d
Wang, Y., Yang, L., Peng, X., & Jin, Z. (2017b). High catalytic activity over novel Mg-Fe/Ti layered double hydroxides (LDHs) for polycarbonate diols (PCDLs): Synthesis, mechanism and application. RSC Advances, 7(56), 35181–35190. https://doi.org/10.1039/c7ra05892f
Wang, J., Liu, X., Yang, M., Han, H., Zhang, S., Ouyang, G., & Han, R. (2021). Removal of tetracycline using modified wheat straw from solution in batch and column modes. Journal of Molecular Liquids, 338, 116698. https://doi.org/10.1016/j.molliq.2021.116698
Weng, B., Fenghua, Xu., Alcoutlabi, M., Mao, Y., & Lozano, K. (2015). Fibrous cellulose membrane mass produced via Forcespinning® for lithium-ion battery separators. Cellulose, 22(2), 1311–1320. https://doi.org/10.1007/s10570-015-0564-8
Wu, Y., Li, X., Zhao, H., Yao, F., Cao, J., Chen, Z., Wang, D., & Yang, Q. (2021). Core-shell structured Cu2O@HKUST-1 heterojunction photocatalyst with robust stability for highly efficient tetracycline hydrochloride degradation under visible light. Chemical Engineering Journal, 426, 131255. https://doi.org/10.1016/j.cej.2021.131255
Xie, Y., Yuan, X., Wu, Z., Zeng, G., Jiang, L., Peng, X., & Li, H. (2019). Adsorption behavior and mechanism of Mg/Fe layered double hydroxide with Fe3O4-carbon spheres on the removal of Pb(II) and Cu(II). Journal of Colloid and Interface Science, 536, 440–55. https://doi.org/10.1016/j.jcis.2018.10.066
Xu, M., & Wei, M. (2018). Layered double hydroxide-based catalysts: Recent advances in preparation, structure, and applications. Advanced Functional Materials, 28(47), 1802943. https://doi.org/10.1002/adfm.201802943
Yang, Z., Jia, S., Zhang, T., Zhuo, N., Dong, Y., Yang, W., & Wang, Y. (2015). How heavy metals impact on flocculation of combined pollution of heavy metals–antibiotics: A comparative study. Separation and Purification Technology, 149, 398–406. https://doi.org/10.1016/j.seppur.2015.06.018
Zhang, Y., Jiao, Z., Yongyou, Hu., Lv, S., Fan, H., Zeng, Y., Jun, Hu., & Wang, M. (2017). Removal of tetracycline and oxytetracycline from water by magnetic Fe3O4@graphene. Environmental Science and Pollution Research, 24(3), 2987–2995. https://doi.org/10.1007/s11356-016-7964-7
Zhang, P., He, T., Chen, H., Li, P., Xiang, M., Ding, N., & Deng, S. (2020). The tetracyclines removal by MgAl layered double oxide in the presence of phosphate or nitrate: Behaviors and mechanism exploration. Journal of Colloid and Interface Science, 578, 124–34. https://doi.org/10.1016/j.jcis.2020.04.122
Zhang, D., He, Q., Hu, X., Zhang, K., Chen, C., & Xue, Y. (2021). Enhanced adsorption for the removal of tetracycline hydrochloride (TC) using ball-milled biochar derived from crayfish shell. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 615, 126254. https://doi.org/10.1016/j.colsurfa.2021.126254
Zhao, J., Gao, F., Sun, Y., Fang, W., Li, X., & Dai, Y. (2021). New use for biochar derived from bovine manure for tetracycline removal. Journal of Environmental Chemical Engineering, 9(4), 105585. https://doi.org/10.1016/j.jece.2021.105585
Author information
Authors and Affiliations
Contributions
All authors contributed to the study conception and design. All authors read and approved the final manuscript. MSM, MCD, and MGLS executed the experiments and manuscript writing; HAA, LM, II, PP, and MAA carried out the manuscript interpretation and corrections.
Corresponding authors
Ethics declarations
Ethical Approval
This material is the authors’ own original work, which has not been previously published elsewhere.
Consent to Participate
Not applied.
Consent for Publication
Not applied.
Competing Interests
The authors declare no competing interests.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Manzar, M.S., Aziz, H.A., Meili, L. et al. Adsorption of Tetracycline onto MgFe-LDH/Cellulose Nanocrystals Structured Composite. Water Air Soil Pollut 234, 291 (2023). https://doi.org/10.1007/s11270-023-06297-6
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-023-06297-6