Abstract
Excessive phosphorus in water causes eutrophication and leads to the ecological unbalance. The main treatment for eutrophication is to remove the phosphorus in aqua system effectively and efficiently. A composite of fly ash (FA) and metal compound was proposed as the effective sorbent for phosphorus removal, attributed to the active metal compositions and stable structure, as well as the wide source availability of economy. Copper and iron were co-precipitated as a bimetallic compound (BM), well adhered onto fly ash, to acquire the composite sorbent of Cu/Fe-BM@FA. Through the characterizations of XPS, FTIR etc., phosphorus adsorption was achieved mainly upon heterogeneous chemisorption and electrostatic attraction. Consequently, from pH 3 to pH 6, phosphorus of 98% on average was removed in solutions of 0 ~ 40 mg P/L, and the maximum adsorption capacity was up to 32.88 mg/g. Promisingly, the composite sorbent of FA and copper/iron bimetallic compound was a potential and economic selection for phosphorus removal.













Similar content being viewed by others
Explore related subjects
Discover the latest articles and news from researchers in related subjects, suggested using machine learning.Data Availability
All data generated during this study are demonstrated in the form of table and/or figure.
References
Abu-Dalo, M., Jaradat, A., Albiss, B. A., & Al-Rawashdeh, N. A. F. (2019). Green synthesis of TiO2 NPs/pristine pomegranate peel extract nanocomposite and its antimicrobial activity for water disinfection. Journal of Environmental Chemical Engineering, 7. https://doi.org/10.1016/j.jece.2019.103370
Akter, J., Islam, M. A., Kibria, K. Q., & Islam, M. A. (2021). Adsorption of phosphate ions on chicken feather hydrochar and hydrochar-soil mixtures. Water, Air, & Soil Pollution, 232. https://doi.org/10.1007/s11270-021-05336-4
Bada, S. O., Potgieter, J. H., & Afolabi, A. S. (2013). Kinetics studies of adsorption and desorption of South African fly ash for some phenolic compounds. Particulate Science and Technology., 31, 1–9. https://doi.org/10.1080/02726351.2011.613897
Bawab, A. A., N. Ghannam, R. A. Abu-Zurayk, F. Odeh and M. A. J. F. E. B. Abu- Da Lo (2018). Olive mill wastewater remediation with granular activated carbon impregnated with active materials. Fresenius Environmental Bulletin, 24, 2118–2126. https://www.webofscience.com/wos/alldb/full-record/WOS:000430372900019
Canımkurbey, B. (2020). Investigation dielectric and morphological properties of fly ash collected from thermal power plant. Asia-Pacific Journal of Chemical Engineering., 15,. https://doi.org/10.1002/apj.2437
Chandraker, N., Jyoti, G., Singh Thakur, R., & Kumar Chaudhari, P. (2021). Removal of fluoride using fly ash adsorbent. IOP Conference Series: Earth and Environmental Science, 597. https://doi.org/10.1088/1755-1315/597/1/012009
Chen, H., W. Zhou, S. Zhu, F. Liu, L. Qin, C. Xu and Z. Wang (2021). Biological nitrogen and phosphorus removal by a phosphorus-accumulating bacteria Acinetobacter sp. strain C-13 with the ability of heterotrophic nitrification-aerobic denitrification. Bioresour Technol, 322,124507. https://doi.org/10.1016/j.biortech.2020.124507
Cheng, G., Li, Q., Su, Z., Sheng, S., & Fu, J. (2018). Preparation, optimization, and application of sustainable ceramsite substrate from coal fly ash/waterworks sludge/oyster shell for phosphorus immobilization in constructed wetlands. Journal of Cleaner Production., 175, 572–581. https://doi.org/10.1016/j.jclepro.2017
Chien, S. H., & Clayton, W. R. (1980). Application of elovich equation to the kinetics of phosphate release and sorption in soils. Soil Science Society of America Journal., 44, 265–268. https://doi.org/10.2136/sssaj1980.03615995004400020013x
Chouyyok, W., Wiacek, R. J., Pattamakomsan, K., Sangvanich, T., Grudzien, R. M., Fryxell, G. E., & Yantasee, W. (2010). Phosphate removal by anion binding on functionalized nanoporous sorbents. Environmental Science and Technology, 44, 3073–3078. https://doi.org/10.1021/es100787m
De Maman, R., Behling, L., da Luz, V. C., Dervanoski, A., Rosa, C. D., & Pasquali, G. D. L. (2022). Oxidation of textile dye through electrocoagulation process using scrap iron electrodes. Water, Air, & Soil Pollution, 233. https://doi.org/10.1007/s11270-022-05564-2
Fan, M., & Brown, R. C. (2002). Comparison of the loss-on-ignition and thermogravimetric analysis techniques in measuring unburned carbon in coal fly ash. Fuel and Energy Abstracts, 43. https://doi.org/10.1016/s0140-6701(02)86209-9
Figueira, P., Henriques, B., Teixeira, F., Afonso, N., Pinto, J., Tavares, D., Vale, C., & Pereira, E. (2022). Potentialities of agro-based wastes to remove Cd, Hg, Pb, and As from contaminated waters. Water, Air, & Soil Pollution, 233. https://doi.org/10.1007/s11270-022-05543-7
Gao, M., Wang, W., Yang, H., & Ye, B.-C. (2020). Efficient removal of fluoride from aqueous solutions using 3D flower-like hierarchical zinc-magnesium-aluminum ternary oxide microspheres. Chemical Engineering Journal, 380. https://doi.org/10.1016/j.cej.2019.122459
Goscianska, J., Ptaszkowska-Koniarz, M., Frankowski, M., Franus, M., Panek, R., & Franus, W. (2018). Removal of phosphate from water by lanthanum-modified zeolites obtained from fly ash. Journal of Colloid and Interface Science, 513, 72–81. https://doi.org/10.1016/j.jcis.2017.11.003
Hermassi, M., Valderrama, C., Moreno, N., Font, O., Querol, X., Batis, N. H., & Cortina, J. L. (2017). Fly ash as reactive sorbent for phosphate removal from treated waste water as a potential slow release fertilizer. Journal of Environmental Chemical Engineering., 5, 160–169. https://doi.org/10.1016/j.jece.2016.11.027
Ifthikar, J., Wang, J., Wang, Q., Wang, T., Wang, H., Khan, A., Jawad, A., Sun, T., Jiao, X., & Chen, Z. (2017). Highly efficient lead distribution by magnetic sewage sludge biochar: Sorption mechanisms and bench applications. Bioresource Technology, 238, 399–406. https://doi.org/10.1016/j.biortech.2017.03.133
Ji, X., Wu, D., Wang, Y., Ge, L., Hong, W., Xue, R., & Wang, B. (2015). Fabrication of lanthanum-based phosphate binder using cross-linked alginate as a carrier. RSC Advances., 5, 55191–55200. https://doi.org/10.1039/c5ra03941j
Jin, H., Lin, L., Meng, X., Wang, L., Huang, Z., Liu, M., Dong, L., Hu, Y., & Crittenden, J. C. (2021). A novel lanthanum-modified copper tailings adsorbent for phosphate removal from water. Chemosphere, 281, 130779. https://doi.org/10.1016/j.chemosphere.2021.130779
Jung, K. W., Hwang, M. J., Jeong, T. U., & Ahn, K. H. (2015a). A novel approach for preparation of modified-biochar derived from marine macroalgae: Dual purpose electro-modification for improvement of surface area and metal impregnation. Bioresource Technology, 191, 342–345. https://doi.org/10.1016/j.biortech.2015.05.052
Jung, K. W., Jeong, T. U., Hwang, M. J., Kim, K., & Ahn, K. H. (2015b). Phosphate adsorption ability of biochar/Mg-Al assembled nanocomposites prepared by aluminum-electrode based electro-assisted modification method with MgCl(2) as electrolyte. Bioresource Technology, 198, 603–610. https://doi.org/10.1016/j.biortech.2015.09.068
Junli, H., Lihua, C., & Zhenye, Z. (2001). Technical note the pattern of ClO2 stabilized by Na2CO3/H2O2. Water Research, 35, 2570–2573. https://doi.org/10.1016/s0043-1354(00)00465-6
Karaca, H., Altıntığ, E., Türker, D., & Teker, M. (2018). An evaluation of coal fly ash as an adsorbent for the removal of methylene blue from aqueous solutions: Kinetic and thermodynamic studies. Journal of Dispersion Science and Technology., 39, 1800–1807. https://doi.org/10.1080/01932691.2018.1462191
Kim, K., Kim, D., Kim, T., Kim, B.-G., Ko, D., Lee, J., Han, Y., Jung, J. C., & Na, H. B. (2019). Synthesis of mesoporous lanthanum hydroxide with enhanced adsorption performance for phosphate removal. RSC Advances., 9, 15257–15264. https://doi.org/10.1039/c9ra00895k
Kong, L., Tian, Y., Pang, Z., Huang, X., Li, M., Yang, R., Li, N., Zhang, J., & Zuo, W. (2019). Synchronous phosphate and fluoride removal from water by 3D rice-like lanthanum-doped La@MgAl nanocomposites. Chemical Engineering Journal., 371, 893–902. https://doi.org/10.1016/j.cej.2019.04.116
Li, X., Shen, S., Xu, Y., Guo, T., Dai, H., & Lu, X. (2021). Application of membrane separation processes in phosphorus recovery: A review. Science of the Total Environment, 767, 144346. https://doi.org/10.1016/j.scitotenv.2020.144346
Liang, M., Yan, L., Wang, D., Cheng, X., Deng, Z., Xu, S., & Li, S. (2020). Novel iron manganese oxide modified mulberry biochar for the adsorption of phosphorus in aqueous solution. Desalination and Water Treatment., 189, 357–366. https://doi.org/10.5004/dwt.2020.25640
Lin, J., He, S., Wang, X., Zhang, H., & Zhan, Y. (2019). Removal of phosphate from aqueous solution by a novel Mg(OH)2/ZrO2 composite: Adsorption behavior and mechanism. Colloids and Surfaces a: Physicochemical and Engineering Aspects., 561, 301–314. https://doi.org/10.1016/j.colsurfa.2018.11.001
Liu, D., Yang, Y., & Zhao, F. (2019). Preparation of adsorbent from fly ash for methylene blue wastewater treatment. IOP Conference Series: Materials Science and Engineering, 490. https://doi.org/10.1088/1757-899x/490/2/022040
Lu, S. G., Bai, S. Q., Zhu, L., & Shan, H. D. (2009). Removal mechanism of phosphate from aqueous solution by fly ash. Journal of Hazardous Materials., 161, 95–101. https://doi.org/10.1016/j.jhazmat.2008.02.123
Mahadevan, H., Krishnan, K. A., Pillai, R. R., & Sudhakaran, S. (2020). Assessment of urban river water quality and developing strategies for phosphate removal from water and wastewaters: Integrated monitoring and mitigation studies. SN Applied Sciences, 2. https://doi.org/10.1007/s42452-020-2571-0
Mahmoodi, N. M. (2013). Nickel ferrite nanoparticle: Synthesis, modification by surfactant and dye removal ability. Water, Air, & Soil Pollution, 224. https://doi.org/10.1007/s11270-012-1419-7
Manto, M. J., Xie, P., Keller, M. A., Liano, W. E., Pu, T., & Wang, C. (2017). Recovery of inorganic phosphorus using copper-substituted ZSM-5. ACS Sustainable Chemistry & Engineering., 5, 6192–6200. https://doi.org/10.1021/acssuschemeng.7b01127
Mazzini, S., Borgonovo, G., Scaglioni, L., Bedussi, F., D’Imporzano, G., Tambone, F., & Adani, F. (2020). Phosphorus speciation during anaerobic digestion and subsequent solid/liquid separation. Science of the Total Environment, 734, 139284. https://doi.org/10.1016/j.scitotenv.2020.139284
Nájera-Martínez, M., Landon-Hernández, G. G., Romero-López, J. P., Domínguez-López, M. L., & Vega-López, A. (2021). Disruption of neurotransmission, membrane potential, and mitochondrial calcium in the brain and spinal cord of nile tilapia elicited by microcystis aeruginosa extract: An uncommon consequence of the eutrophication process. Water, Air, & Soil Pollution, 233. https://doi.org/10.1007/s11270-021-05480-x
Nejati, K., Davary, S., & Saati, M. (2013). Study of 2,4-dichlorophenoxyacetic acid (2,4-D) removal by Cu-Fe-layered double hydroxide from aqueous solution. Applied Surface Science., 280, 67–73. https://doi.org/10.1016/j.apsusc.2013.04.086
Onutai, S., Kobayashi, T., Thavorniti, P., & Jiemsirilers, S. (2018). Removal of Pb(2+), Cu(2+), Ni(2+), Cd(2+) from Wastewater using fly ash based geopolymer as an adsorbent. Key Engineering Materials., 773, 373–378. https://doi.org/10.4028/www.scientific.net/KEM.773.373
Peng, L., Dai, H., Wu, Y., Peng, Y., & Lu, X. (2018). A comprehensive review of the available media and approaches for phosphorus recovery from wastewater. Water, Air, & Soil Pollution, 229. https://doi.org/10.1007/s11270-018-3706-4
Samiullah, M., Aslam, Z., Rana, A. G., Abbas, A., & Ahmad, W. (2018). Alkali-activated boiler fly ash for Ni(II) removal: Characterization and parametric study. Water, Air, & Soil Pollution, 229. https://doi.org/10.1007/s11270-018-3758-5
Siwek, H., Bartkowiak, A., Wlodarczyk, M., & Sobecka, K. (2016). Removal of phosphate from aqueous solution using alginate/iron (III) chloride capsules: A laboratory study. Water, Air, & Soil Pollution., 227, 427. https://doi.org/10.1007/s11270-016-3128-0
Soliman, A. M., Elwy, H. M., Thiemann, T., Majedi, Y., Labata, F. T., & Al-Rawashdeh, N. A. F. (2016). Removal of Pb(II) ions from aqueous solutions by sulphuric acid-treated palm tree leaves. Journal of the Taiwan Institute of Chemical Engineers., 58, 264–273. https://doi.org/10.1016/j.jtice.2015.05.035
Tu, Y.-J., & You, C.-F. (2014). Phosphorus adsorption onto green synthesized nano-bimetal ferrites: Equilibrium, kinetic and thermodynamic investigation. Chemical Engineering Journal., 251, 285–292. https://doi.org/10.1016/j.cej.2014.04.036
Ugurlu, M., Gurses, A., Yalcin, M., & Dogar, C. (2005). Removal of phenolic and lignin compounds from bleached Kraft mill effluent by fly ash and sepiolite. Adsorption, 11, 87–97. https://doi.org/10.1007/s10450-005-1096-6
Wang, H., Tian, Z., Wang, H., & Yan, Q. (2020b). Optimization and reaction kinetics analysis for phosphorus removal in struvite precipitation process. Water Environment Research, 92, 1162–1172. https://doi.org/10.1002/wer.1311
Wang, L., Z. Zhang, J. Zhang and L. Zhang (2016). Magnetic solid-phase extraction using nanoporous three dimensional graphene hybrid materials for high-capacity enrichment and simultaneous detection of nine bisphenol analogs from water sample. Journal of Chromatography A, 1463, 1–10. https://doi.org/10.1016/j.chroma.2016.08.003
Wang, C., R. Yang and H. Wang (2020a). Synthesis of ZIF-8/fly ash composite for adsorption of Cu(2+), Zn(2+) and Ni(2+) from aqueous solutions. Materials (Basel). 13. https://doi.org/10.3390/ma13010214
Wu, B., J. Wan, Y. Zhang, B. Pan and I. M. C. Lo (2020). Selective phosphate removal from water and wastewater using sorption: Process fundamentals and removal mechanisms. Environmental Science & Technology, 54, 50–66. https://doi.org/10.1021/acs.est.9b05569
Xiong, W., & Peng, J. (2010). Laboratory-scale investigation of ferrihydrite-modified diatomite as a phosphorus co-precipitant. Water, Air, & Soil Pollution., 215, 645–654. https://doi.org/10.1007/s11270-010-0506-x
Xue, R., Xu, J., Gu, L., Pan, L., & He, Q. (2018). Study of phosphorus removal by using sponge iron adsorption. Water, Air, & Soil Pollution, 229. https://doi.org/10.1007/s11270-018-3753-x
Yang, F., Zhang, S., Sun, Y., Tsang, D. C. W., Cheng, K., & Ok, Y. S. (2019). Assembling biochar with various layered double hydroxides for enhancement of phosphorus recovery. Journal of Hazardous Materials., 365, 665–673. https://doi.org/10.1016/j.jhazmat.2018.11.047
Yokoi, T., Tatsumi, T., & Yoshitake, H. (2003). Selective selenate adsorption on cationated amino-functionalized MCM-41. Bulletin of the Chemical Society of Japan., 76, 2225–2232. https://doi.org/10.1246/bcsj.76.2225
Yokoi, T., Tatsumi, T., & Yoshitake, H. (2004). Fe(3+) coordinated to amino-functionalized MCM-41: An adsorbent for the toxic oxyanions with high capacity, resistibility to inhibiting anions, and reusability after a simple treatment. Journal of Colloid and Interface Science, 274, 451–457. https://doi.org/10.1016/j.jcis.2004.02.037
Yoshitake, H., Yokoi, T., & Tatsumi, T. (2003). Adsorption behavior of arsenate at transition metal cations captured by amino-functionalized mesoporous silicas. Chemistry of Materials., 15, 1713–1721. https://doi.org/10.1021/cm0218007
You, Y., Vance, G. F., & Zhao, H. (2001). Selenium adsorption on Mg–Al and Zn–Al layered double hydroxides. Applied Clay Science., 20, 13–25. https://doi.org/10.1016/s0169-1317(00)00043-0
Yu, P., Xue, Y., Gao, F., Liu, Z., Cheng, X., & Yang, K. (2016). Phosphorus removal from aqueous solution by pre- or post-modified biochars derived from agricultural residues. Water, Air, & Soil Pollution, 227. https://doi.org/10.1007/s11270-016-3066-x
Zhang, G., Ren, Z., Zhang, X., & Chen, J. (2013a). Nanostructured iron(III)-copper(II) binary oxide: A novel adsorbent for enhanced arsenic removal from aqueous solutions. Water Research, 47, 4022–4031. https://doi.org/10.1016/j.watres.2012.11.059
Zhang, M., Gao, B., Yao, Y., & Inyang, M. (2013b). Phosphate removal ability of biochar/MgAl-LDH ultra-fine composites prepared by liquid-phase deposition. Chemosphere, 92, 1042–1047. https://doi.org/10.1016/j.chemosphere.2013.02.050
Zhang, X., Zhang, X.-Q., Yu, H.-B., Song, H.-L., & Du, M.-X. (2020). Phosphorus removal from wastewater by electrocoagulation with magnetized iron particle anode. Water, Air, & Soil Pollution, 231. https://doi.org/10.1007/s11270-020-04869-4
Zheng, X., Sun, W., Wei, N., Bian, T., Zhang, Y., Li, L., Zhang, Y., Li, Z., & Ou, H. (2021). Bionic-inspired La–Zn(4,4′-dipy)(OAc)2/bacterial cellulose composite membrane for efficient separation of nitrogen and phosphorus in water. Materials Chemistry and Physics, 274. https://doi.org/10.1016/j.matchemphys.2021.125162
Funding
The authors received support of the National Natural Science Foundation of China (21506028), the National Key Research and Development Program of China (2019YFE0119200), and the Fundamental Research Funds for the Central Universities (DUT20LK43).
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Competing 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.
Rights and permissions
About this article
Cite this article
Ge, W., Li, S., Jiang, M. et al. Cu/Fe Bimetallic Modified Fly Ash: An Economical Adsorbent for Enhanced Phosphorus Removal from Aqueous Solutions. Water Air Soil Pollut 233, 182 (2022). https://doi.org/10.1007/s11270-022-05628-3
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-022-05628-3


