Abstract
Different aqueous selenium species including selenite, selenate, and selenocyanate, can be harmful to both humans and other life forms. Considering this, the present study investigated the application of Mg-Fe-LDH nanomaterial adsorbent for the removal of aqueous selenite, selenate, and selenocyanate species. The research examined the removal efficiency of selenite, selenate, and selenocyanate under a varying set of competitive conditions including Mg-Fe-LDH dosage (0.5–1.5) g/l, Mg-Fe-LDH calcination temperature (0–500 °C), and concentration of selenium species (2.5–7.5 ppm). The respective experimental results showed a higher removal for the selenite and selenate species as compared to the selenocyanate species. Also, the Freundlich isotherm provided a good fit both for selenite and selenocyanate uptake whereas for selenate the Langmuir isotherm provided a better fit. Furthermore, the study found that the removal of selenite and selenocyanate followed the pseudo-first-order and pseudo-second-order models, respectively, while both models fitted well with selenate. This work also employed response surface methodology (RSM) and back-propagation artificial neural network (BPANN) based modeling techniques to predict the removal efficiency of respective selenium species. The modeling results demonstrated that the BPANN method exhibited a higher accuracy in predicting selenium species removal as compared to the RSM technique. To that end, the BPANN-based models yielded R2 values of 0.9894, 0.9709, and 0.9568 for selenite, selenate, and selenocyanate, respectively. In contrast, the RSM methodology showed lower R2 values, i.e., 0.9464 for selenite, 0.9002 for selenate, and 0.8225 for selenocyanate.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
Data Availability
All Data used are included in the paper.
References
Abdelkader, N., Bentouami, A., Derriche, Z., Bettahar, N., & de Ménorval, L. C. (2011). Synthesis and characterization of Mg-Fe layer double hydroxides and its application on adsorption of Orange G from aqueous solution. Chemical Engineering Journal, 169(1–3), 231–238. https://doi.org/10.1016/j.cej.2011.03.019
Ahmed, S. A. A., & Vohra, M. S. (2021). Treatment of aqueous selenocyanate (SeCN-) using combined TiO2 photocatalysis and 2-line ferrihydrite adsorption. Desalination and Water Treatment, 211, 267–279. https://doi.org/10.5004/dwt.2021.26589
Alaejos, M. S., & Romero, C. D. (1995). Analysis of selenium in body fluids : A review, 227–257. https://doi.org/10.1021/cr00033a009
Bandara, P. C., Perez, J. V. D., Nadres, E. T., Nannapaneni, R. G., Krakowiak, K. J., & Rodrigues, D. F. (2019). Graphene oxide nanocomposite hydrogel beads for removal of selenium in contaminated water. ACS Applied Polymer Materials, 1(10), 2668–2679. https://doi.org/10.1021/acsapm.9b00612
Bingöl, D., Hercan, M., Elevli, S., & Kiliç, E. (2012). Comparison of the results of response surface methodology and artificial neural network for the biosorption of lead using black cumin. Bioresource Technology, 112, 111–115. https://doi.org/10.1016/j.biortech.2012.02.084
Chen, M. L., & An, M. I. (2012). Selenium adsorption and speciation with Mg-FeCO3 layered double hydroxides loaded cellulose fibre. Talanta, 95, 31–35. https://doi.org/10.1016/j.talanta.2012.03.038
Chubar, N. (2014). EXAFS and FTIR studies of selenite and selenate sorption by alkoxide-free sol-gel generated Mg-Al-CO3 layered double hydroxide with very labile interlayer anions. Journal of Materials Chemistry A, 2(38), 15995–16007. https://doi.org/10.1039/c4ta03463e
Das, J., Das, D., Dash, G. P., & Parida, K. M. (2002). Studies on Mg/Fe hydrotalcite-like-compound (HTLC): I. Removal of inorganic selenite (SeO32-) from aqueous medium. Journal of Colloid and Interface Science, 251(1), 26–32. https://doi.org/10.1006/jcis.2002.8319
Das, J., Sairam Patra, B., Baliarsingh, N., & Parida, K. M. (2007). Calcined Mg-Fe-CO3 LDH as an adsorbent for the removal of selenite. Journal of Colloid and Interface Science, 316(2), 216–223. https://doi.org/10.1016/j.jcis.2007.07.082
Dorraji, M. S., Amani-Ghadim, A. R., Hanifehpour, Y., Woo Joo, S., Figoli, A., Carraro, M., & Tasselli, F. (2017). Performance of chitosan based nanocomposite hollow fibers in the removal of selenium(IV) from water. Chemical Engineering Research and Design, 117, 309–317. https://doi.org/10.1016/j.cherd.2016.10.043
Elmoubarki, R., Zahra, F., Elhalil, A., Tounsadi, H., & Barka, N. (2017). Ni / Fe and Mg / Fe layered double hydroxides and their calcined derivatives : Preparation, characterization, and application on textile dyes. Integrative Medicine Research, 6(3), 271–283. https://doi.org/10.1016/j.jmrt.2016.09.007
Gallup, D. L. (1997). Removal of selenocyanate in water by precipitation : characterization of copper - selenium precipitate by X-ray diffraction, infrared, and X-ray absorption spectroscopy. 31(4), 968–976. https://doi.org/10.1021/es960138a
Ghahremani, P., Nezamzadeh-Ejhieh, A., & Vakili, M. H. (2023). A novel biodegradable magnetically/recyclable cellulose-based adsorbent: synthesis, characterization, and experimental design toward Cd(II) removal. Water, Air, & Soil Pollution, 234(3), 158. https://doi.org/10.1007/s11270-023-06176-0
Gonzalez, C. M., Hernandez, J., Peralta-Videa, J. R., Botez, C. E., Parsons, J. G., & Gardea-Torresdey, J. L. (2012). Sorption kinetic study of selenite and selenate onto a high and low pressure aged iron oxide nanomaterial. Journal of Hazardous Materials, 211–212, 138–145. https://doi.org/10.1016/j.jhazmat.2011.08.023
Hong, S. H., Lyonga, F. N., Kang, J. K., Lee, E. C., Sanghyun, J. F., Hong, S. J., Park, S. J. (2020). Synthesis of Fe-impregnated biochar from food waste for Selenium(VI). Chemosphere, 252. https://doi.org/10.1016/j.chemosphere.2020.126475
Hussaini, M., & Vohra, M. (2022). LDH-TiO2 Composite for Selenocyanate (SeCN−) Photocatalytic degradation: Characterization, treatment efficiency, reaction intermediates and modeling. Nanomaterials, 12(12). https://doi.org/10.3390/nano12122035
Jadhav, A. S., Ali Amrani, M., Singh, S. K., Al-Fatesh, A. S., Bansiwal, A., Srikanth, V. V. S. S., & Labhasetwar, N. K. (2020). γ-FeOOH and γ-FeOOH decorated multi-layer graphene: Potential materials for selenium(VI) removal from water. Journal of Water Process Engineering, 37(September 2019), 101396. https://doi.org/10.1016/j.jwpe.2020.101396
Kazeem, T. S., Labaran, B. A., Ahmed, H., Mohammed, T., Essa, M.H., Al-Suwaiyan, M.S., Vohra, M.S. (2019). Treatment of aqueous selenocyanate anions using electrocoagulation. International Journal of Electrochemical Science, 14, 10538–10564. https://doi.org/10.20964/2019.11.51
Kumar, S., Manokar, S. N., Thirunavookarasu, N., Nivethitha, V., Nidhusri, T. N., & Niranjana, T. (2022). Characterization of Power Ultrasound Modified Kappaphycus alvarezii Biosorbent and its Modeling by Artificial Neural Networks. Water, Air, & Soil Pollution, 233(7), 234. https://doi.org/10.1007/s11270-022-05690-x
Labaran, B. A., & Vohra, M. S. (2017). Solar photocatalytic removal of selenite, selenate, and selenocyanate species. Clean - Soil, Air, Water, 45(10). https://doi.org/10.1002/clen.201600268
Labaran, B. A., & Vohra, M. S. (2014). Photocatalytic removal of selenite and selenate species: Effect of EDTA and other process variables. Environmental Technology (United Kingdom), 35(9), 1091–1100. https://doi.org/10.1080/09593330.2013.861857
Labaran, B. A., & Vohra, M. S. (2016). Application of activated carbon produced from phosphoric acid-based chemical activation of oil fly ash for the removal of some charged aqueous phase dyes: Role of surface charge, adsorption kinetics, and modeling. Desalination and Water Treatment, 57(34), 16034–16052. https://doi.org/10.1080/19443994.2015.1074118
Labaran, B. A., & Vohra, M. S. (2018). Competitive adsorption of selenite [Se(IV)], selenate [Se(VI)] and selenocyanate [SeCN–] species onto TiO2: Experimental findings and surface complexation modeling. Desalination and Water Treatment, 124, 267–278. https://doi.org/10.5004/dwt.2018.22742
Li, D., Yan, W., Guo, X., Tian, Q., Xu, Z., & Zhu, L. (2020a). Removal of selenium from caustic solution by adsorption with Ca[sbnd]Al layered double hydroxides. Hydrometallurgy, 191(June 2019), 105231. https://doi.org/10.1016/j.hydromet.2019.105231
Li, P., Chen, P., Liu, Z., Nie, S., Wang, X., Wang, G., et al. (2020b). Highly efficient elimination of uranium from wastewater with facilely synthesized Mg-Fe layered double hydroxides: Optimum preparation conditions and adsorption kinetics. Annals of Nuclear Energy, 140, 107140. https://doi.org/10.1016/j.anucene.2019.107140
Ma, B., Fernandez-Martinez, A., Grangeon, S., Tournassat, C., Findling, N., Carrero, S., et al. (2018). Selenite uptake by Ca-Al LDH: A description of intercalated anion coordination geometries. Environmental Science and Technology, 52(3), 1624–1632. https://doi.org/10.1021/acs.est.7b04644
Mandal, S., Mayadevi, S., & Kulkarni, B. D. (2009). Adsorption of aqueous selenite [Se(IV)] species on synthetic layered double Hydroxide Materials. Industrial and Engineering Chemistry Research, 48(17), 7893–7898. https://doi.org/10.1021/ie900136s
Meng, X., Bang, S., & Korfiatis, G. P. (2002). Removal of selenocyanate from water using elemental iron. Water Research, 36(15), 3867–3873. https://doi.org/10.1016/S0043-1354(02)00086-6
Mourabet, M., Rhilassi, A. E., Boujaady, H. E., Hamri, R. E., & Taitai, A. (2015). Removal of fluoride from aqueous solution by adsorption on hydroxyapatite (HAp) using response surface methodology. Journal of Saudi Chemical Society, 19, 603–615. https://doi.org/10.1016/j.jscs.2012.03.003
Nabavi, E., Shamskilani, M., Dezvareh, G. A., & Darban, A. K. (2023). ANN-based modeling of combined O3/H2O2 oxidation, and activated carbon adsorption treatment system: Forest polluting site leachate. Water, Air, & Soil Pollution, 234(2), 86. https://doi.org/10.1007/s11270-023-06099-w
Nishimura, T., Hashimoto, H., & Nakayama, M. (2007). Removal of selenium(VI) from aqueous solution with polyamine-type weakly basic ion exchange resin. Separation Science and Technology, 42(14), 3155–3167. https://doi.org/10.1080/01496390701513107
Ostrowski, S. R., Wilbur, S., Chou, C. H. S. J., Pohl, H. R., Stevens, Y. W., & Allred, P. M. (1999). Agency for toxic substances and disease registry’s 1997 priority list of hazardous substances. Latent effects—carcinogenesis, neurotoxicology, and developmental deficits in humans and animals. Toxicology and Industrial Health, 15(7), 602–644. https://doi.org/10.1177/074823379901500702
Riaz, M., & Mehmood, K. T. (2012). Selenium in human health and disease: A review. Journal of Postgraduate Medical Institute, 26(2), 120–133. https://doi.org/10.1089/ars.2010.3275
Rives, V., Arco, M., & Martín, C. (2014). Applied Clay Science Intercalation of drugs in layered double hydroxides and their controlled release: A review. Applied Clay Science, 88–89, 239–269. https://doi.org/10.1016/j.clay.2013.12.002
Sahan, T., Ceylan, H., Sahiner, N., Aktas, N. (2010). Optimization of removal conditions of copper ions from aqueous solutions by Trametes versicolor. Bioresource Technology, 4520–4526. https://doi.org/10.1016/j.biortech.2010.01.105
Séby, F., Potin-Gautier, M., Giffaut, E., & Donard, O. F. X. (1998). Assessing the speciation and the biogeochemical processes affecting the mobility of selenium from a geological repository of radioactive wastes to the biosphere. Analusis, 26(5), 193–198. https://doi.org/10.1051/analusis:1998134
Shan, R. R., Yan, L. G., Yang, K., Hao, Y. F., & Du, B. (2015). Adsorption of Cd(II) by Mg-Al-CO3- and magnetic Fe3O4/Mg-Al-CO3-layered double hydroxides: Kinetic, isothermal, thermodynamic and mechanistic studies. Journal of Hazardous Materials, 299, 42–49. https://doi.org/10.1016/j.jhazmat.2015.06.003
Shi, K., Ye, Y., Guo, N., Guo, Z., & Wu, W. (2014). Evaluation of Se(IV) removal from aqueous solution by GMZ Na-bentonite: Batch experiment and modeling studies. Journal of Radioanalytical and Nuclear Chemistry, 299(1), 583–589. https://doi.org/10.1007/s10967-013-2807-1
Shojaeimehr, T., Rahimpour, F., Khadivi, M. A., & Sadeghi, M. (2014). A modeling study by response surface methodology (RSM) and artificial neural network (ANN) on Cu2+ adsorption optimization using light expended clay aggregate (LECA). Journal of Industrial and Engineering Chemistry, 20(3), 870–880. https://doi.org/10.1016/j.jiec.2013.06.017
Simmons, D. B. D., & Wallschläger, D. (2005). A critical review of the biogeochemistry and ecotoxicology of selenium in lotic and lentic environments. Environmental Toxicology and Chemistry, 24(6), 1331–1343. https://doi.org/10.1897/04-176R.1
Sun, X., Imai, T., Sekine, M., Higuchi, T., Yamamoto, K., & Akagi, K. (2013). Adsorption of phosphate by calcinated Mg-Fe layered double hydroxide. Journal of Water and Environment Technology, 11(2), 111–120. https://doi.org/10.2965/jwet.2013.111
Torres, J., Pintos, V., Domínguez, S., Kremer, C., & Kremer, E. (2010). Selenite and selenate speciation in natural waters: Interaction with divalent metal ions. Journal of Solution Chemistry, 39(1), 1–10. https://doi.org/10.1007/s10953-009-9491-3
Turan, N. G., Mesci, B., & Ozgonenel, O. (2011). Artificial neural network (ANN) approach for modeling Zn(II) adsorption from leachate using a new biosorbent. Chemical Engineering Journal, 173(1), 98–105. https://doi.org/10.1016/j.cej.2011.07.042
Tyagi, S., Bashir, M., Mohan, C., & Annachhatre, A. (2022). Characterization of pine residues from himalayan region and their use as copper adsorbent. Water, Air, & Soil Pollution, 233(6), 226. https://doi.org/10.1007/s11270-022-05624-7
Vohra, M. S. (2015). Selenocyanate (SeCN-) contaminated waste-water treatment using TiO2 photocatalysis: SeCN- complex destruction, intermediates formation, and removal of selenium species. 24(3), 1108–1118. https://www.prt-parlar.de/download/
Vohra, M. S., & Labaran, B. A. (2020). Photocatalytic treatment of mixed selenocyanate and phenol streams: Process modeling, optimization, and kinetics. Environmental Progress and Sustainable Energy, 39(4), 1–11. https://doi.org/10.1002/ep.13401
Wang, Q., Tay, H. H., Ng, D. J. W., Chen, L., Liu, Y., Chang, J., et al. (2010). The effect of trivalent cations on the performance of Mg-M-CO3 layered double hydroxides for high-temperature CO2 capture. Chemsuschem, 3(8), 965–973. https://doi.org/10.1002/cssc.201000099
Xia, X., Ling, L., & Zhang, W. X. (2017). Solution and surface chemistry of the Se(IV)-Fe(0) reactions: Effect of initial solution pH. Chemosphere, 168, 1597–1603. https://doi.org/10.1016/j.chemosphere.2016.11.150
Xie, Y., Dong, H., Zeng, G., Zhang, L., Cheng, Y., Hou, K., et al. (2017). The comparison of Se(IV) and Se(VI) sequestration by nanoscale zero-valent iron in aqueous solutions: The roles of solution chemistry. Journal of Hazardous Materials, 338, 306–312. https://doi.org/10.1016/j.jhazmat.2017.05.053
Xu, L., & Huang, Y. (2019). A novel layered double hydroxide coupled with zero valent iron system for selenate removal under anaerobic condition: Batch and continuous studies. Chemical Engineering Journal, 359(August 2018), 1166–1174. https://doi.org/10.1016/j.cej.2018.11.061
Yigit, N. O., & Tozum, S. (2012). Removal of selenium species from waters using various surface-modified natural particles and waste materials. Clean - Soil, Air, Water, 40(7), 735–745. https://doi.org/10.1002/clen.201100740
Zhu, Y., Sengupta, A. K., Ramana, A. (1992). Ligand exchange for anionic solutes. 17, 229–237. https://doi.org/10.1016/0923-1137(92)90155-U
Acknowledgements
The authors are thankful to the Civil and Environmental Department at the King Fahd University of Petroleum & Minerals (KFUPM) for providing the lab facilities and also the Deanship of Research Oversight and Coordination at KFUPM (DROC-KFUPM) for support through project number SB191028.
Funding
The authors are thankful to the Deanship of Research Oversight and Coordination at KFUPM (DROC-KFUPM) for support through project number SB191028.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of Interest
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.
Supplementary Information
Below is the link to the electronic supplementary material.
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
Ibrahim, A.I.A., Vohra, M.S. Mg-Fe-LDH for Aquatic Selenium Treatment: Adsorption, RSM Modeling, and Machine Learning Neural Network. Water Air Soil Pollut 234, 433 (2023). https://doi.org/10.1007/s11270-023-06444-z
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-023-06444-z